ALBERT

Description: We present a Lagrangian convective transport scheme developed for global chemistry and transport models, which considers the variable residence time that an air parcel spends in convection. This is particularly important for accurately simulating the tropospheric chemistry of short-lived species, e.g., for determining the time available for heterogeneous chemical processes on the surface of cloud droplets. In current Lagrangian convective transport schemes air parcels are stochastically redistributed within a fixed time step according to estimated probabilities for convective entrainment as well as the altitude of detrainment. We introduce a new scheme that extends this approach by modeling the variable time that an air parcel spends in convection by estimating vertical updraft velocities. Vertical updraft velocities are obtained by combining convective mass fluxes from meteorological analysis data with a parameterization of convective area fraction profiles. We implement two different parameterizations: a parameterization using an observed constant convective area fraction profile and a parameterization that uses randomly drawn profiles to allow for variability. Our scheme is driven by convective mass fluxes and detrainment rates that originate from an external convective parameterization, which can be obtained from meteorological analysis data or from general circulation models. We study the effect of allowing for a variable time that an air parcel spends in convection by performing simulations in which our scheme is implemented into the trajectory module of the ATLAS chemistry and transport model and is driven by the ECMWF ERA-Interim reanalysis data. In particular, we show that the redistribution of air parcels in our scheme conserves the vertical mass distribution and that the scheme is able to reproduce the convective mass fluxes and detrainment rates of ERA-Interim. We further show that the estimated vertical updraft velocities of our scheme are able to reproduce wind profiler measurements performed in Darwin, Australia, for velocities larger than 0.6 m s−1. SO2 is used as an example to show that there is a significant effect on species mixing ratios when modeling the time spent in convective updrafts compared to a redistribution of air parcels in a fixed time step. Furthermore, we perform long-time global trajectory simulations of radon-222 and compare with aircraft measurements of radon activity.

Description: A multi-model intercomparison of halogenated very short-lived substances (TransCom-VSLS): linking oceanic emissions and tropospheric transport for a reconciled estimate of the stratospheric source gas injection of bromine R. Hossaini, P. K. Patra, A. A. Leeson, G. Krysztofiak, N. L. Abraham, S. J. Andrews, A. T. Archibald, J. Aschmann, E. L. Atlas, D. A. Belikov, H. Bönisch, L. J. Carpenter, S. Dhomse, M. Dorf, A. Engel, W. Feng, S. Fuhlbrügge, P. T. Griffiths, N. R. P. Harris, R. Hommel, T. Keber, K. Krüger, S. T. Lennartz, S. Maksyutov, H. Mantle, G. P. Mills, B. Miller, S. A. Montzka, F. Moore, M. A. Navarro, D. E. Oram, K. Pfeilsticker, J. A. Pyle, B. Quack, A. D. Robinson, E. Saikawa, A. Saiz-Lopez, S. Sala, B.-M. Sinnhuber, S. Taguchi, S. Tegtmeier, R. T. Lidster, C. Wilson, and F. Ziska Atmos. Chem. Phys., 16, 9163-9187, doi:10.3334/CDIAC/hippo_012, 2016 The first concerted multi-model intercomparison of halogenated very short-lived substances (VSLS) has been performed, within the framework of the ongoing Atmospheric Tracer Transport Model Intercomparison Project (TransCom). Eleven global models or model variants participated (nine chemical transport models and two chemistry–climate models) by simulating the major natural bromine VSLS, bromoform (CHBr 3 ) and dibromomethane (CH 2 Br 2 ), over a 20-year period (1993–2012). Except for three model simulations, all others were driven offline by (or nudged to) reanalysed meteorology. The overarching goal of TransCom-VSLS was to provide a reconciled model estimate of the stratospheric source gas injection (SGI) of bromine from these gases, to constrain the current measurement-derived range, and to investigate inter-model differences due to emissions and transport processes. Models ran with standardised idealised chemistry, to isolate differences due to transport, and we investigated the sensitivity of results to a range of VSLS emission inventories. Models were tested in their ability to reproduce the observed seasonal and spatial distribution of VSLS at the surface, using measurements from NOAA's long-term global monitoring network, and in the tropical troposphere, using recent aircraft measurements – including high-altitude observations from the NASA Global Hawk platform. The models generally capture the observed seasonal cycle of surface CHBr 3 and CH 2 Br 2 well, with a strong model–measurement correlation ( r   ≥  0.7) at most sites. In a given model, the absolute model–measurement agreement at the surface is highly sensitive to the choice of emissions. Large inter-model differences are apparent when using the same emission inventory, highlighting the challenges faced in evaluating such inventories at the global scale. Across the ensemble, most consistency is found within the tropics where most of the models (8 out of 11) achieve best agreement to surface CHBr 3 observations using the lowest of the three CHBr 3 emission inventories tested (similarly, 8 out of 11 models for CH 2 Br 2 ). In general, the models reproduce observations of CHBr 3 and CH 2 Br 2 obtained in the tropical tropopause layer (TTL) at various locations throughout the Pacific well. Zonal variability in VSLS loading in the TTL is generally consistent among models, with CHBr 3 (and to a lesser extent CH 2 Br 2 ) most elevated over the tropical western Pacific during boreal winter. The models also indicate the Asian monsoon during boreal summer to be an important pathway for VSLS reaching the stratosphere, though the strength of this signal varies considerably among models. We derive an ensemble climatological mean estimate of the stratospheric bromine SGI from CHBr 3 and CH 2 Br 2 of 2.0 (1.2–2.5) ppt,  ∼  57 % larger than the best estimate from the most recent World Meteorological Organization (WMO) Ozone Assessment Report. We find no evidence for a long-term, transport-driven trend in the stratospheric SGI of bromine over the simulation period. The transport-driven interannual variability in the annual mean bromine SGI is of the order of ±5 %, with SGI exhibiting a strong positive correlation with the El Niño–Southern Oscillation (ENSO) in the eastern Pacific. Overall, our results do not show systematic differences between models specific to the choice of reanalysis meteorology, rather clear differences are seen related to differences in the implementation of transport processes in the models.

Description: A multi-model intercomparison of halogenated very short-lived substances (TransCom-VSLS): linking oceanic emissions and tropospheric transport for a reconciled estimate of the stratospheric source gas injection of bromine R. Hossaini, P. K. Patra, A. A. Leeson, G. Krysztofiak, N. L. Abraham, S. J. Andrews, A. T. Archibald, J. Aschmann, E. L. Atlas, D. A. Belikov, H. Bönisch, L. J. Carpenter, S. Dhomse, M. Dorf, A. Engel, W. Feng, S. Fuhlbrügge, P. T. Griffiths, N. R. P. Harris, R. Hommel, T. Keber, K. Krüger, S. T. Lennartz, S. Maksyutov, H. Mantle, G. P. Mills, B. Miller, S. A. Montzka, F. Moore, M. A. Navarro, D. E. Oram, K. Pfeilsticker, J. A. Pyle, B. Quack, A. D. Robinson, E. Saikawa, A. Saiz-Lopez, S. Sala, B.-M. Sinnhuber, S. Taguchi, S. Tegtmeier, R. T. Lidster, C. Wilson, and F. Ziska Atmos. Chem. Phys., 16, 9163-9187, doi:10.3334/CDIAC/hippo_012, 2016 The first concerted multi-model intercomparison of halogenated very short-lived substances (VSLS) has been performed, within the framework of the ongoing Atmospheric Tracer Transport Model Intercomparison Project (TransCom). Eleven global models or model variants participated (nine chemical transport models and two chemistry–climate models) by simulating the major natural bromine VSLS, bromoform (CHBr 3 ) and dibromomethane (CH 2 Br 2 ), over a 20-year period (1993–2012). Except for three model simulations, all others were driven offline by (or nudged to) reanalysed meteorology. The overarching goal of TransCom-VSLS was to provide a reconciled model estimate of the stratospheric source gas injection (SGI) of bromine from these gases, to constrain the current measurement-derived range, and to investigate inter-model differences due to emissions and transport processes. Models ran with standardised idealised chemistry, to isolate differences due to transport, and we investigated the sensitivity of results to a range of VSLS emission inventories. Models were tested in their ability to reproduce the observed seasonal and spatial distribution of VSLS at the surface, using measurements from NOAA's long-term global monitoring network, and in the tropical troposphere, using recent aircraft measurements – including high-altitude observations from the NASA Global Hawk platform. The models generally capture the observed seasonal cycle of surface CHBr 3 and CH 2 Br 2 well, with a strong model–measurement correlation ( r   ≥  0.7) at most sites. In a given model, the absolute model–measurement agreement at the surface is highly sensitive to the choice of emissions. Large inter-model differences are apparent when using the same emission inventory, highlighting the challenges faced in evaluating such inventories at the global scale. Across the ensemble, most consistency is found within the tropics where most of the models (8 out of 11) achieve best agreement to surface CHBr 3 observations using the lowest of the three CHBr 3 emission inventories tested (similarly, 8 out of 11 models for CH 2 Br 2 ). In general, the models reproduce observations of CHBr 3 and CH 2 Br 2 obtained in the tropical tropopause layer (TTL) at various locations throughout the Pacific well. Zonal variability in VSLS loading in the TTL is generally consistent among models, with CHBr 3 (and to a lesser extent CH 2 Br 2 ) most elevated over the tropical western Pacific during boreal winter. The models also indicate the Asian monsoon during boreal summer to be an important pathway for VSLS reaching the stratosphere, though the strength of this signal varies considerably among models. We derive an ensemble climatological mean estimate of the stratospheric bromine SGI from CHBr 3 and CH 2 Br 2 of 2.0 (1.2–2.5) ppt,  ∼  57 % larger than the best estimate from the most recent World Meteorological Organization (WMO) Ozone Assessment Report. We find no evidence for a long-term, transport-driven trend in the stratospheric SGI of bromine over the simulation period. The transport-driven interannual variability in the annual mean bromine SGI is of the order of ±5 %, with SGI exhibiting a strong positive correlation with the El Niño–Southern Oscillation (ENSO) in the eastern Pacific. Overall, our results do not show systematic differences between models specific to the choice of reanalysis meteorology, rather clear differences are seen related to differences in the implementation of transport processes in the models.

Description: The first concerted multi-model intercomparison of halogenated very short-lived substances (VSLS) has been performed, within the framework of the ongoing Atmospheric Tracer Transport Model Intercomparison Project (TransCom). Eleven global models or model variants participated, simulating the major natural bromine VSLS, bromoform (CHBr3) and dibromomethane (CH2Br2), over a 20-year period (1993-2012). The overarching goal of TransCom-VSLS was to provide a reconciled model estimate of the stratospheric source gas injection (SGI) of bromine from these gases, to constrain the current measurement-derived range, and to investigate inter-model differences due to emissions and transport processes.Models ran with standardised idealised chemistry, to isolate differences due to transport, and we investigated the sensitivity of results to a range of VSLS emission inventories. Models were tested in their ability to reproduce the observed seasonal and spatial distribution of VSLS at the surface, using measurements from NOAA’s long-term global monitoring network, and in the tropical troposphere, using recent aircraft measurements - including high altitude observations from the NASA Global Hawk platform. The models generally capture the seasonal cycle of surface CHBr3 and CH2Br2 well, with a strong model-measurement correlation (r ≥ 0.7) and a low sensitivity to the choice of emission inventory, at most sites. In a given model, the absolute model-measurement agreement is highly sensitive to the choice of emissions and inter-model differences are also apparent, even when using the same inventory, highlighting the challenges faced in evaluating such inventories at the global scale. Across the ensemble, most consistency is found within the tropics where most of the models (8 out of 11) achieve optimal agreement to surface CHBr3 observations using the lowest of the three CHBr3 emission inventories tested (similarly, 8 out of 11 models for CH2 Br2). In general, the models are able to reproduce well observations of CHBr3 and CH2 Br2 obtained in the tropical tropopause layer (TTL) at various locations throughout the Pacific. Zonal variability in VSLS loading in the TTL is generally consistent among models, with CHBr3 (and to a lesser extent CH2 Br2) most elevated over the tropical West Pacific during boreal winter. The models also indicate the Asian Monsoon during boreal summer to be an important pathway for VSLS reaching the stratosphere, though the strength of this signal varies considerably among models. We derive an ensemble climatological mean estimate of the stratospheric bromine SGI from CHBr3 and CH2 Br2 of 2.0 (1.2-2.5) ppt, ≫ 57% larger than the best estimate from the most recent World Meteorological Organization (WMO) Ozone Assessment Report. We find no evidence for a long-term, transport-driven trend in the stratospheric SGI of bromine over the simulation period. However, transport-driven inter-annual variability in the annual mean bromine SGI is of the order of a ±5%, with SGI exhibiting a strong positive correlation with ENSO in the East Pacific.

Description: The first concerted multi-model intercomparison of halogenated very short-lived substances (VSLS) has been performed, within the framework of the ongoing Atmospheric Tracer Transport Model Intercomparison Project (TransCom). Eleven global models or model variants participated (nine chemical transport models and two chemistry–climate models) by simulating the major natural bromine VSLS, bromoform (CHBr3) and dibromomethane (CH2Br2), over a 20-year period (1993–2012). Except for three model simulations, all others were driven offline by (or nudged to) reanalysed meteorology. The overarching goal of TransCom-VSLS was to provide a reconciled model estimate of the stratospheric source gas injection (SGI) of bromine from these gases, to constrain the current measurement-derived range, and to investigate inter-model differences due to emissions and transport processes. Models ran with standardised idealised chemistry, to isolate differences due to transport, and we investigated the sensitivity of results to a range of VSLS emission inventories. Models were tested in their ability to reproduce the observed seasonal and spatial distribution of VSLS at the surface, using measurements from NOAA's long-term global monitoring network, and in the tropical troposphere, using recent aircraft measurements – including high-altitude observations from the NASA Global Hawk platform. The models generally capture the observed seasonal cycle of surface CHBr3 and CH2Br2 well, with a strong model–measurement correlation (r  ≥  0.7) at most sites. In a given model, the absolute model–measurement agreement at the surface is highly sensitive to the choice of emissions. Large inter-model differences are apparent when using the same emission inventory, highlighting the challenges faced in evaluating such inventories at the global scale. Across the ensemble, most consistency is found within the tropics where most of the models (8 out of 11) achieve best agreement to surface CHBr3 observations using the lowest of the three CHBr3 emission inventories tested (similarly, 8 out of 11 models for CH2Br2). In general, the models reproduce observations of CHBr3 and CH2Br2 obtained in the tropical tropopause layer (TTL) at various locations throughout the Pacific well. Zonal variability in VSLS loading in the TTL is generally consistent among models, with CHBr3 (and to a lesser extent CH2Br2) most elevated over the tropical western Pacific during boreal winter. The models also indicate the Asian monsoon during boreal summer to be an important pathway for VSLS reaching the stratosphere, though the strength of this signal varies considerably among models. We derive an ensemble climatological mean estimate of the stratospheric bromine SGI from CHBr3 and CH2Br2 of 2.0 (1.2–2.5) ppt,  ∼  57 % larger than the best estimate from the most recent World Meteorological Organization (WMO) Ozone Assessment Report. We find no evidence for a long-term, transport-driven trend in the stratospheric SGI of bromine over the simulation period. The transport-driven interannual variability in the annual mean bromine SGI is of the order of ±5 %, with SGI exhibiting a strong positive correlation with the El Niño–Southern Oscillation (ENSO) in the eastern Pacific. Overall, our results do not show systematic differences between models specific to the choice of reanalysis meteorology, rather clear differences are seen related to differences in the implementation of transport processes in the models.

Description: Idealized models or emulators of volcanic aerosol forcing have been widely used to reconstruct the spatiotemporal evolution of past volcanic forcing. However, existing models, including the most recently developed Easy Volcanic Aerosol (EVA; Toohey et al., doi: 10.5194/gmd‐2016‐83), (i) do not account for the height of injection of volcanic SO urn:x-wiley:jgrd:media:jgrd55987:jgrd55987-math-0001; (ii) prescribe a vertical structure for the forcing; and (iii) are often calibrated against a single eruption. We present a new idealized model, EVA_H, that addresses these limitations. Compared to EVA, EVA_H makes predictions of the global mean stratospheric aerosol optical depth that are (i) similar for the 1979–1998 period characterized by the large and high‐altitude tropical SO urn:x-wiley:jgrd:media:jgrd55987:jgrd55987-math-0002 injections of El Chichón (1982) and Mount Pinatubo (1991); (ii) significantly improved for the 1998–2015 period characterized by smaller eruptions with a large variety of injection latitudes and heights. Compared to EVA, the sensitivity of volcanic forcing to injection latitude and height in EVA_H is much more consistent with results from climate models that include interactive aerosol chemistry and microphysics, even though EVA_H remains less sensitive to eruption latitude than the latter models. We apply EVA_H to investigate potential biases and uncertainties in EVA‐based volcanic forcing data sets from phase 6 of the Coupled Model Intercomparison Project (CMIP6). EVA and EVA_H forcing reconstructions do not significantly differ for tropical high‐altitude volcanic injections. However, for high‐latitude or low‐altitude injections, our reconstructed forcing is significantly lower. This suggests that volcanic forcing in CMIP6 last millenium experiments may be overestimated for such eruptions.

Description: Three volcanic arcs have been the source of New Zealand's volcanic activity since the Neogene: Northland arc, Coromandel Volcanic Zone (CVZ) and Taupō Volcanic Zone (TVZ). The eruption chronology for the Quaternary, sourced by the TVZ, is well studied and established, whereas the volcanic evolution of the precursor arc systems, like the CVZ (central activity c. 18 to 2 Ma), is poorly known due to limited accessibility to, or identification of, onshore volcanic deposits and their sources. Here, we investigate the marine tephra record of the Neogene, mostly sourced by the CVZ, of cores from IODP Exp. 375 (Sites U1520 and U1526), ODP Leg 181 (Sites 1123, 1124 and 1125), IODP Leg 329 (Site U1371) and DSDP Leg 90 (Site 594) offshore of New Zealand. In total, we identify 306 primary tephra layers in the marine sediments. Multi-approach age models (e.g. biostratigraphy, zircon ages) are used in combination with geochemical fingerprinting (major and trace element compositions) and the stratigraphic context of each marine tephra layer to establish 168 tie-lines between marine tephra layers from different holes and sites. Following this approach, we identify 208 explosive volcanic events in the Neogene between c. 17.5 and 2.6 Ma. This is the first comprehensive study of New Zealand's Neogene explosive volcanism established from tephrochronostratigraphic studies, which reveals continuous volcanic activity between c. 12 and 2.6 Ma with an abrupt compositional change at c. 4.5 Ma, potentially associated with the transition from CVZ to TVZ. Key Points New Zealand's Neogene explosive volcanism based on the marine tephra record Geochemical fingerprinting of marine tephra layers across the study area to establish volcanic events Insights into geochemical variations with time, repose times and spatiotemporal distribution

Description: Springtime Arctic mixed-phase convection over open water in the Fram Strait as observed during the recent ACLOUD (Arctic CLoud Observations Using airborne measurements during polar Day) field campaign is simulated at turbulence-resolving resolutions. The first objective is to assess the skill of large-eddy simulation (LES) in reproducing the observed mixed-phase convection. The second goal is to then use the model to investigate how aerosol modulates the way in which turbulent mixing and clouds transform the low-level air mass. The focus lies on the low-level thermal structure and lapse rate, the heating efficiency of turbulent entrainment, and the low-level energy budget. A composite case is constructed based on data collected by two research aircraft on 18 June 2017. Simulations are evaluated against independent datasets, showing that the observed thermodynamic, cloudy, and turbulent states are well reproduced. Sensitivity tests on cloud condensation nuclei (CCN) concentration are then performed, covering a broad range between pristine polar and polluted continental values. We find a significant response in the resolved mixed-phase convection, which is in line with previous LES studies. An increased CCN substantially enhances the depth of convection and liquid cloud amount, accompanied by reduced surface precipitation. Initializing with the in situ CCN data yields the best agreement with the cloud and turbulence observations, a result that prioritizes its measurement during field campaigns for supporting high-resolution modeling efforts. A deeper analysis reveals that CCN significantly increases the efficiency of radiatively driven entrainment in warming the boundary layer. The marked strengthening of the thermal inversion plays a key role in this effect. The low-level heat budget shifts from surface driven to radiatively driven. This response is accompanied by a substantial reduction in the surface energy budget, featuring a weakened flow of solar radiation into the ocean. Results are interpreted in the context of air–sea interactions, air mass transformations, and climate feedbacks at high latitudes.

Description: The high variability of aerosol particle concentrations, sizes and chemical composition makes their description challenging in atmospheric models. Aerosol–cloud interaction studies are usually focused on the activation of accumulation mode particles as cloud condensation nuclei (CCN). However, under specific conditions Aitken mode particles can also contribute to the number concentration of cloud droplets (Nd), leading to large uncertainties in predicted cloud properties on a global scale. We perform sensitivity studies with an adiabatic cloud parcel model to constrain conditions under which Aitken mode particles contribute to Nd. The simulations cover wide ranges of aerosol properties, such as total particle number concentration, hygroscopicity (κ) and mode diameters for accumulation and Aitken mode particles. Building upon the previously suggested concept of updraft (w)- and aerosol-limited regimes of cloud droplet formation, we show that activation of Aitken mode particles does not occur in w-limited regimes of accumulation mode particles. The transitional range between the regimes is broadened when Aitken mode particles contribute to Nd, as aerosol limitation requires much higher w than for aerosol size distributions with accumulation mode particles only. In the transitional regime, Nd is similarly dependent on w and κ. Therefore, we analyze the sensitivity of Nd to κ, ξ(κ), as a function of w to identify the value combinations above which Aitken mode particles can affect Nd. As ξ(κ) shows a minimum when the smallest activated particle size is in the range of the “Hoppel minimum” (0.06 µm ≤ Dmin ≤0.08 µm), the corresponding (w–κ) pairs can be considered a threshold level above which Aitken mode particles have significant impact on Nd. This threshold is largely determined by the number concentration of accumulation mode particles and by the Aitken mode diameter. Our analysis of these thresholds results in a simple parametric framework and criterion to identify aerosol and updraft conditions under which Aitken mode particles are expected to affect aerosol–cloud interactions. Our results confirm that Aitken mode particles likely do not contribute to Nd in polluted air masses (urban, biomass burning) at moderate updraft velocities (w≤3 m s−1) but may be important in deep convective clouds. Under clean conditions, such as in the Amazon, the Arctic and remote ocean regions, hygroscopic Aitken mode particles can act as CCN at updrafts of w

Description: Submarine groundwater discharge (SGD) is a globally important process supplying nutrients and trace elements to the coastal environment, thus playing a pivotal role in sustaining marine primary productivity. Along with nutrients, groundwater also contains allochthonous microbes that are discharged from the terrestrial subsurface into the sea. Currently, little is known about the interactions between groundwater‐borne and coastal seawater microbial populations, and groundwater microbes' role upon introduction to coastal seawater populations. Here, we investigated seawater microbial abundance, activity and diversity in a site strongly influenced by SGD. In addition, through laboratory‐controlled bottle incubations, we mimicked different mixing scenarios between groundwater and seawater. Our results demonstrate that the addition of 0.1 μm filtered groundwater stimulated heterotrophic activity and increased microbial abundance compared to control coastal seawater, whereas 0.22 μm filtration treatments induced primary productivity and Synechococcus growth. 16S rRNA gene sequencing showed a strong shift from a SAR11‐rich community in the control samples to Rhodobacteraceae dominance in the 〈0.1 μm treatment, in agreement with Rhodobacteraceae enrichment in the SGD field site. These results suggest that microbes delivered by SGD may affect the abundance, activity and diversity of intrinsic microbes in coastal seawater, highlighting the cryptic interplay between groundwater and seawater microbes in coastal environments, which has important implications for carbon cycling. Plain Language Summary Submarine groundwater discharge (SGD) is an important process where groundwater flows into the ocean along the coast. When the groundwater mixes with seawater, the microbes from both sources interact with each other, which can impact the diversity, activity, and amount of microbes in the coastal environment. Currently, little is known about how groundwater‐borne microbes affect marine microbial populations. Our research shows that when groundwater microbes are removed before mixing groundwater with seawater, the abundance and activity of certain microbes that consume organic matter significantly increase. Additionally, we noticed a significant difference in the types of microbes present between the sites where SGD occurs versus background (uninfluenced) coastal water, especially in terms of the microbes that consume organic matter. Overall, this study suggests that there is a connection between groundwater and seawater microbes, which can influence the delicate balance between organisms that produce carbon and those that consume it. This has important implications for how carbon cycles globally. Key Points Groundwater discharge into the coastal zone delivers both nutrients and allochthonous microbes Groundwater microbes interact with seawater populations, by which affecting the delicate autotroph‐heterotroph balance Subterranean microbial processes are key drivers of food webs, potentially affecting biogenic carbon fluxes in the ocean

Description: Climate trends in the Antarctic region remain poorly characterized, owing to the brevity and scarcity of direct climate observations and the large magnitude of interannual to decadal-scale climate variability. Here, within the framework of the PAGES Antarctica2k working group, we build an enlarged database of ice core water stable isotope records from Antarctica, consisting of 112 records. We produce both unweighted and weighted isotopic (δ18O) composites and temperature reconstructions since 0 CE, binned at 5- and 10-year resolution, for seven climatically distinct regions covering the Antarctic continent. Following earlier work of the Antarctica2k working group, we also produce composites and reconstructions for the broader regions of East Antarctica, West Antarctica and the whole continent. We use three methods for our temperature reconstructions: (i) a temperature scaling based on the δ18O–temperature relationship output from an ECHAM5-wiso model simulation nudged to ERA-Interim atmospheric reanalyses from 1979 to 2013, and adjusted for the West Antarctic Ice Sheet region to borehole temperature data, (ii) a temperature scaling of the isotopic normalized anomalies to the variance of the regional reanalysis temperature and (iii) a composite-plus-scaling approach used in a previous continent-scale reconstruction of Antarctic temperature since 1 CE but applied to the new Antarctic ice core database. Our new reconstructions confirm a significant cooling trend from 0 to 1900 CE across all Antarctic regions where records extend back into the 1st millennium, with the exception of the Wilkes Land coast and Weddell Sea coast regions. Within this long-term cooling trend from 0 to 1900 CE, we find that the warmest period occurs between 300 and 1000 CE, and the coldest interval occurs from 1200 to 1900 CE. Since 1900 CE, significant warming trends are identified for the West Antarctic Ice Sheet, the Dronning Maud Land coast and the Antarctic Peninsula regions, and these trends are robust across the distribution of records that contribute to the unweighted isotopic composites and also significant in the weighted temperature reconstructions. Only for the Antarctic Peninsula is this most recent century-scale trend unusual in the context of natural variability over the last 2000 years. However, projected warming of the Antarctic continent during the 21st century may soon see significant and unusual warming develop across other parts of the Antarctic continent. The extended Antarctica2k ice core isotope database developed by this working group opens up many avenues for developing a deeper understanding of the response of Antarctic climate to natural and anthropogenic climate forcings. The first long-term quantification of regional climate in Antarctica presented herein is a basis for data–model comparison and assessments of past, present and future driving factors of Antarctic climate.

Description: Key Points: - A new CHBr3 emission inventory based on natural and anthropogenic sources suggests that the latter account for 12%–28% of the global emissions - In the NH, new anthropogenic estimates increase known natural CHBr3 emissions by up to 70.5%, leading to higher atmospheric CHBr3 levels - At the NH extratropical tropopause, CHBr3 is enhanced by 0.9 ppt Br due to anthropogenic sources thus doubling natural CHBr3 abundances Bromoform (CHBr3) contributes to stratospheric ozone depletion but is not regulated under the Montreal Protocol due to its short lifetime and large natural sources. Here, we show that anthropogenic sources contribute significantly to the amount of CHBr3 transported into the Northern Hemisphere (NH) extratropical stratosphere. We present a new CHBr3 emission inventory comprised of natural and anthropogenic sources, with the latter estimated from ship ballast, power plant cooling and desalination plant brine water. Including anthropogenic sources in the new inventory increases CHBr3 emissions by up to 31.5% globally and 70.5% in the NH. In consequence, atmospheric CHBr3 is also significantly higher, especially over the NH extratropics during boreal winter. Here anthropogenic sources enhance bromine at the tropopause by 0.9 ppt Br, thus doubling natural CHBr3 abundances. For some latitudes, tropopause bromine increases by 2.4 ppt Br suggesting significant contributions of anthropogenic CHBr3 to the NH lowermost stratosphere.

Description: Assessment of cloud supersaturation by aerosol particle and cloud condensation nuclei (CCN) measurements Atmospheric Measurement Techniques Discussions, 6, 10021-10056, 2013 Author(s): M. L. Krüger, S. Mertes, T. Klimach, Y. Cheng, H. Su, J. Schneider, M. O. Andreae, U. Pöschl, and D. Rose In this study we show how size-resolved measurements of aerosol particles and cloud condensation nuclei (CCN) can be used to characterize the supersaturation of water vapor in a cloud. The method was developed and applied for the investigation of a cloud event during the ACRIDICON-Zugspitze campaign (17 September to 4 October 2012) at the high-alpine research station Schneefernerhaus (German Alps, 2650 m a.s.l.). Number size distributions of total and interstitial aerosol particles were measured with a scanning mobility particle sizer (SMPS), and size-resolved CCN efficiency spectra were recorded with a CCN counter system operated at different supersaturation levels. During the evolution of a cloud, aerosol particles are exposed to different supersaturation levels. We outline and compare different estimates for the lower and upper bounds ( S low , S high ) and the average value ( S avg ) of peak supersaturation encountered by the particles in the cloud. For the investigated cloud event, we derived S low ≈ 0.19–0.25%, S high ≈ 0.90–1.64% and S avg ≈ 0.38–0.84%. Estimates of S low , S high and S avg based on aerosol size distribution data require specific knowledge or assumptions of aerosol hygroscopicity, which are not required for the derivation of S low and S avg from the size-resolved CCN efficiency spectra.

Description: In this study we show how size-resolved measurements of aerosol particles and cloud condensation nuclei (CCN) can be used to characterize the supersaturation of water vapor in a cloud. The method was developed and applied for the investigation of a cloud event during the ACRIDICON-Zugspitze campaign (17 September to 4 October 2012) at the high-alpine research station Schneefernerhaus (German Alps, 2650 m a.s.l.). Number size distributions of total and interstitial aerosol particles were measured with a scanning mobility particle sizer (SMPS), and size-resolved CCN efficiency spectra were recorded with a CCN counter system operated at different supersaturation levels. During the evolution of a cloud, aerosol particles are exposed to different supersaturation levels. We outline and compare different estimates for the lower and upper bounds (Slow, Shigh) and the average value (Savg) of peak supersaturation encountered by the particles in the cloud. For the investigated cloud event, we derived Slow ≈ 0.19–0.25%, Shigh ≈ 0.90–1.64% and Savg ≈ 0.38–0.84%. Estimates of Slow, Shigh and Savg based on aerosol size distribution data require specific knowledge or assumptions of aerosol hygroscopicity, which are not required for the derivation of Slow and Savg from the size-resolved CCN efficiency spectra.

Description: Assessment of cloud supersaturation by size-resolved aerosol particle and cloud condensation nuclei (CCN) measurements Atmospheric Measurement Techniques, 7, 2615-2629, 2014 Author(s): M. L. Krüger, S. Mertes, T. Klimach, Y. F. Cheng, H. Su, J. Schneider, M. O. Andreae, U. Pöschl, and D. Rose In this study we show how size-resolved measurements of aerosol particles and cloud condensation nuclei (CCN) can be used to characterize the supersaturation of water vapor in a cloud. The method was developed and applied during the ACRIDICON-Zugspitze campaign (17 September to 4 October 2012) at the high-Alpine research station Schneefernerhaus (German Alps, 2650 m a.s.l.). Number size distributions of total and interstitial aerosol particles were measured with a scanning mobility particle sizer (SMPS), and size-resolved CCN efficiency spectra were recorded with a CCN counter system operated at different supersaturation levels. During the evolution of a cloud, aerosol particles are exposed to different supersaturation levels. We outline and compare different estimates for the lower and upper bounds ( S low , S high ) and the average value ( S avg ) of peak supersaturation encountered by the particles in the cloud. A major advantage of the derivation of S low and S avg from size-resolved CCN efficiency spectra is that it does not require the specific knowledge or assumptions about aerosol hygroscopicity that are needed to derive estimates of S low , S high , and S avg from aerosol size distribution data. For the investigated cloud event, we derived S low ≈ 0.07–0.25%, S high ≈ 0.86–1.31% and S avg ≈ 0.42–0.68%.

Description: In this study we show how size-resolved measurements of aerosol particles and cloud condensation nuclei (CCN) can be used to characterize the supersaturation of water vapor in a cloud. The method was developed and applied during the ACRIDICON-Zugspitze campaign (17 September to 4 October 2012) at the high-Alpine research station Schneefernerhaus (German Alps, 2650 m a.s.l.). Number size distributions of total and interstitial aerosol particles were measured with a scanning mobility particle sizer (SMPS), and size-resolved CCN efficiency spectra were recorded with a CCN counter system operated at different supersaturation levels. During the evolution of a cloud, aerosol particles are exposed to different supersaturation levels. We outline and compare different estimates for the lower and upper bounds (Slow, Shigh) and the average value (Savg) of peak supersaturation encountered by the particles in the cloud. A major advantage of the derivation of Slow and Savg from size-resolved CCN efficiency spectra is that it does not require the specific knowledge or assumptions about aerosol hygroscopicity that are needed to derive estimates of Slow, Shigh, and Savg from aerosol size distribution data. For the investigated cloud event, we derived Slow ≈ 0.07–0.25%, Shigh ≈ 0.86–1.31% and Savg ≈ 0.42–0.68%.

Description: A major stratospheric sudden warming (SSW) in January 2009 was the strongest and most prolonged on record. Aura Microwave Limb Sounder (MLS) observations are used to provide an overview of dynamics and transport during the 2009 SSW, and to compare with the intense, long-lasting SSW in January 2006. The Arctic polar vortex split during the 2009 SSW, whereas the 2006 SSW was a vortex displacement event. Winds reversed to easterly more rapidly and reverted to westerly more slowly in 2009 than in 2006. More mixing of trace gases out of the vortex during the decay of the vortex fragments, and less before the fulfillment of major SSW criteria, was seen in 2009 than in 2006; persistent well-defined fragments of vortex and anticyclone air were more prevalent in 2009. The 2009 SSW had a more profound impact on the lower stratosphere than any previously observed SSW, with no significant recovery of the vortex in that region. The stratopause breakdown and subsequent reformation at very high altitude, accompanied by enhanced descent into a rapidly strengthening upper stratospheric vortex, were similar in 2009 and 2006. Many differences between 2006 and 2009 appear to be related to the different character of the SSWs in the two years.

Description: Biogenic halocarbons from the Peruvian upwelling region as tropospheric halogen source Helmke Hepach, Birgit Quack, Susann Tegtmeier, Anja Engel, Astrid Bracher, Steffen Fuhlbrügge, Luisa Galgani, Elliot L. Atlas, Johannes Lampel, Udo Frieß, and Kirstin Krüger Atmos. Chem. Phys., 16, 12219-12237, doi:10.5194/acp-16-12219-2016, 2016 We present surface seawater measurements of bromo- and iodocarbons, which are involved in numerous atmospheric processes such as tropospheric and stratospheric ozone chemistry, from the highly productive Peruvian upwelling. By combining trace gas measurements, characterization of organic matter and phytoplankton species, and tropospheric modelling, we show that large amounts of iodocarbons produced from the pool of organic matter may contribute strongly to local tropospheric iodine loading.

Description: Biogenic halocarbons from the Peruvian upwelling region as tropospheric halogen source Helmke Hepach, Birgit Quack, Susann Tegtmeier, Anja Engel, Astrid Bracher, Steffen Fuhlbrügge, Luisa Galgani, Elliot L. Atlas, Johannes Lampel, Udo Frieß, and Kirstin Krüger Atmos. Chem. Phys., 16, 12219-12237, doi:10.5194/acp-16-12219-2016, 2016 We present surface seawater measurements of bromo- and iodocarbons, which are involved in numerous atmospheric processes such as tropospheric and stratospheric ozone chemistry, from the highly productive Peruvian upwelling. By combining trace gas measurements, characterization of organic matter and phytoplankton species, and tropospheric modelling, we show that large amounts of iodocarbons produced from the pool of organic matter may contribute strongly to local tropospheric iodine loading.

Description: Halocarbons, halogenated short-chained hydrocarbons, are produced naturally in the oceans by biological and chemical processes. They are emitted from surface seawater into the atmosphere, where they take part in numerous chemical processes such as ozone destruction and the oxidation of mercury and dimethyl sulfide. Here we present oceanic and atmospheric halocarbon data for the Peruvian upwelling obtained during the M91 cruise onboard the research vessel Meteor in December 2012. Surface waters during the cruise were characterized by moderate concentrations of bromoform (CHBr3) and dibromomethane (CH2Br2) correlating with diatom biomass derived from marker pigment concentrations, which suggests this phytoplankton group as likely source. Concentrations measured for the iodinated compounds methyl iodide (CH3I) of up to 35.4 pmol L−1, chloroiodomethane (CH2ClI) of up to 58.1 pmol L−1 and diiodomethane (CH2I2) of up to 32.4 pmol L−1 in water samples were much higher than previously reported for the tropical Atlantic upwelling systems. Iodocarbons also correlated with the diatom biomass and even more significantly with dissolved organic matter (DOM) components measured in the surface water. Our results suggest a biological source of these compounds as significant driving factor for the observed large iodocarbon concentrations. Elevated atmospheric mixing ratios of CH3I (up to 3.2 ppt), CH2ClI (up to 2.5 ppt) and CH2I2 (3.3 ppt) above the upwelling were correlated with seawater concentrations and high sea-to-air fluxes. The enhanced iodocarbon production in the Peruvian upwelling contributed significantly to tropospheric iodine levels.

Description: Halocarbons are produced naturally in the oceans by biological and chemical processes. They are emitted from surface seawater into the atmosphere, where they take part in numerous chemical processes such as ozone destruction and the oxidation of mercury and dimethyl sulfide. Here we present oceanic and atmospheric halocarbon data for the Peruvian upwelling zone obtained during the M91 cruise onboard the research vessel METEOR in December 2012. Surface waters during the cruise were characterized by moderate concentrations of bromoform (CHBr3) and dibromomethane (CH2Br2) correlating with diatom biomass derived from marker pigment concentrations, which suggests this phytoplankton group is a likely source. Concentrations measured for the iodinated compounds methyl iodide (CH3I) of up to 35.4 pmol L−1, chloroiodomethane (CH2ClI) of up to 58.1 pmol L−1 and diiodomethane (CH2I2) of up to 32.4 pmol L−1 in water samples were much higher than previously reported for the tropical Atlantic upwelling systems. Iodocarbons also correlated with the diatom biomass and even more significantly with dissolved organic matter (DOM) components measured in the surface water. Our results suggest a biological source of these compounds as a significant driving factor for the observed large iodocarbon concentrations. Elevated atmospheric mixing ratios of CH3I (up to 3.2 ppt), CH2ClI (up to 2.5 ppt) and CH2I2 (3.3 ppt) above the upwelling were correlated with seawater concentrations and high sea-to-air fluxes. During the first part of the cruise, the enhanced iodocarbon production in the Peruvian upwelling contributed significantly to tropospheric iodine levels, while this contribution was considerably smaller during the second part.

Description: A site at the gas hydrate stability limit was investigated offshore northwestern Svalbard to study methane transport in sediment. The site was characterized by chemosynthetic communities (sulfur bacteria mats, tubeworms) and gas venting. Sediments were sampled with in‐situ porewater collectors and by gravity coring followed by analyses of porewater constituents, sediment and carbonate geochemistry, and microbial activity, taxonomy, and lipid biomarkers. Sulfide and alkalinity concentrations showed concentration maxima in near‐surface sediments at the bacterial mat and deeper maxima at the gas vent site. Sediments at the periphery of the chemosynthetic field were characterized by two sulfate‐methane transition zones (SMTZ) at ~204 and 45 cm depth, where activity maxima of microbial anaerobic oxidation of methane (AOM) with sulfate were found. Amplicon sequencing and lipid biomarker indicate that AOM at the SMTZs was mediated by ANME‐1 archaea. A 1D numerical transport reaction model suggests that the deeper SMTZ‐1 formed on centennial scale by vertical advection of methane, while the shallower SMTZ‐2 could only be reproduced by non‐vertical methane injections starting on decadal scale. Model results were supported by age distribution of authigenic carbonates, showing youngest carbonates within SMTZ‐2. We propose that non‐vertical methane injection was induced by increasing blockage of vertical transport or formation of sediment fractures. Our study further suggests that the methanotrophic response to the non‐vertical methane injection was commensurate with new methane supply. This finding provides new information about for the response time and efficiency of the benthic methane filter in environments with fluctuating methane transport.

Description: Direct dimethyl sulfide (DMS) flux measurements using eddy covariance have shown a suppression of gas transfer at medium to high wind speed. However, not all eddy covariance measurements show evidence of this suppression. Processes, such as wave-wind interaction and surfactants, have been postulated to cause this suppression. We measured DMS and carbon dioxide eddy covariance fluxes during the Asian summer monsoon in the western tropical Indian Ocean (July and August 2014). Both fluxes and their respective gas transfer velocities show signs of a gas transfer suppression above 10 m/s. Using a wind-wave interaction, we describe a flow separation process that could be responsible for a suppression of gas transfer. As a result we provide a Reynolds number-based parameterization, which states the likelihood of a gas transfer suppression for this cruise and previously published gas transfer data. Additionally, we compute the difference in the gas transfer velocities of DMS and CO2 to estimate the bubble-mediated gas transfer using a hybrid model with three whitecap parameterizations.

Description: Oceanic dimethyl sulfide (DMS) is of interest due to its critical influence on atmospheric sulfur compounds in the marine atmosphere and its hypothesized significant role in global climate. High-resolution shipboard underway measurements of surface seawater DMS and the partial pressure of carbon dioxide (pCO2) were conducted in the Atlantic Ocean and Indian Ocean sectors of the Southern Ocean (SO), the southeast Indian Ocean, and the northwest Pacific Ocean from February to April 2014 during the 30th Chinese Antarctic Research Expedition. The SO, particularly in the region south of 58°S, had the highest mean surface seawater DMS concentration of 4.1 ± 8.3 nM (ranged from 0.1 to 73.2 nM) and lowest mean seawater pCO2 level of 337 ± 50 μatm (ranged from 221 to 411 μatm) over the entire cruise. Significant variations of surface seawater DMS and pCO2 in the seasonal ice zone (SIZ) of SO were observed, which are mainly controlled by biological process and sea ice activity. We found a significant negative relationship between DMS and pCO2 in the SO SIZ using 0.1° resolution, [DMS] seawater = -0.160 [pCO2] seawater + 61.3 (r2 = 0.594, n = 924, p 〈 0.001). We anticipate that the relationship may possibly be utilized to reconstruct the surface seawater DMS climatology in the SO SIZ. Further studies are necessary to improve the universality of this approach. Key Points: • The characteristics of surface water DMS and pCO2 distributions from the Southern Ocean to northwest Pacific Ocean are investigated • The correlations between DMS, pCO2, and environmental parameters are analyzed • Anticorrelation between DMS and pCO2 is found in the seasonal ice zone of the Southern Ocean

Description: Monthly zonal mean climatologies of atmospheric measurements from satellite instruments can have biases due to the non-uniform sampling of the atmosphere by the instruments. We characterize potential sampling biases in stratospheric trace gas climatologies of the Stratospheric Processes and their Role in Climate (SPARC) Data Initiative using chemical fields from a chemistry climate model simulation and sampling patterns from 16 satellite-borne instruments. The exercise is performed for the long-lived stratospheric trace gases O3 and H2O. Monthly sample biases for O3 exceed 10% for many instruments in the high latitude stratosphere and in the upper troposphere/lower stratosphere, while annual mean sampling biases reach values of up to 20% in the same regions for some instruments. Sampling biases for H2O are generally smaller than for O3, although still notable in the upper troposphere/lower stratosphere and Southern Hemisphere high latitudes. The most important mechanism leading to monthly sampling bias is the non-uniform temporal sampling of many instruments, i.e., the fact that for many instruments, monthly means are produced from measurements which span less than the full month in question. Similarly, annual mean sampling biases are well explained by non-uniformity in the month-to-month sampling by different instruments. Non-uniform sampling in latitude and longitude are shown to also lead to non-negligible sampling biases, which are most relevant for climatologies which are otherwise free of sampling biases due to non-uniform temporal sampling.

Description: Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign Atmospheric Chemistry and Physics, 15, 8847-8869, 2015 Author(s): E. F. Mikhailov, G. N. Mironov, C. Pöhlker, X. Chi, M. L. Krüger, M. Shiraiwa, J.-D. Förster, U. Pöschl, S. S. Vlasenko, T. I. Ryshkevich, M. Weigand, A. L. D. Kilcoyne, and M. O. Andreae In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in central Siberia (61° N, 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical compositions of aerosol particles were analyzed by x-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38 % of particulate matter (PM) in the accumulation mode and coarse mode, respectively. The water-soluble fraction of organic matter was estimated to be 52 and 8 % of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34 % in the accumulation mode vs. ~ 47 % in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5–99.4 % RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same relative humidity (RH), starting at ~ 70 %, while efflorescence occurred at different humidities, i.e., at ~ 35 % RH for submicron particles vs. ~ 50 % RH for supermicron particles. This ~ 15 % RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5–99.4 % RH range. Based on KIM, the volume-based hygroscopicity parameter, κ v , was calculated. The κ v,ws value related to the water-soluble (ws) fraction was estimated to be ~ 0.15 for the accumulation mode and ~ 0.36 for the coarse mode, respectively. The obtained κ v,ws for the accumulation mode is in good agreement with earlier data reported for remote sites in the Amazon rain forest (κ v ≈ 0.15) and a Colorado mountain forest (κ v ≈ 0.16 ). We used the Zdanovskii–Stokes–Robinson (ZSR) mixing rule to predict the chemical composition dependent hygroscopicity, κ v,p . The obtained κ v,p values overestimate the experimental FDHA-KIM-derived κ v,ws by factors of 1.8 and 1.5 for the accumulation and coarse modes, respectively. This divergence can be explained by incomplete dissolution of the hygroscopic inorganic compounds resulting from kinetic limitations due to a sparingly soluble organic coating. The TEM and STXM-NEXAFS results indicate that aged submicron (〉 300 nm) and supermicron aerosol particles possess core–shell structures with an inorganic core, and are enriched in organic carbon at the mixed particle surface. The direct FDHA kinetic studies provide a bulk diffusion coefficient of water of ~ 10 −12 cm 2 s −1 indicating a semi-solid state of the organic-rich phase leading to kinetic limitations of water uptake and release during hydration and dehydration cycles. Overall, the present ZOTTO data set, obtained in the growing season, has revealed a strong influence of organic carbon on the hygroscopic properties of the ambient aerosols. The sparingly soluble organic coating controls hygroscopic growth, phase transitions, and microstructural rearrangement processes. The observed kinetic limitations can strongly influence the outcome of experiments performed on multi-second timescales, such as the commonly applied HTDMA (Hygroscopicity Tandem Differential Mobility Analyzer) and CCNC (Cloud Condensation Nuclei Counter) measurements.

Description: Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign Atmospheric Chemistry and Physics Discussions, 15, 7837-7893, 2015 Author(s): E. F. Mikhailov, G. N. Mironov, C. Pöhlker, X. Chi, M. L. Krüger, M. Shiraiwa, J.-D. Förster, U. Pöschl, S. S. Vlasenko, T. I. Ryshkevich, M. Weigand, A. L. D. Kilcoyne, and M. O. Andreae In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical composition of aerosol particles were analyzed by X-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38% of PM in the accumulation mode and coarse mode, respectively. The water soluble fraction of organic matter was estimated to be 52 and 8% of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ∼34% in the accumulation vs. ∼47% in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5–99.4% RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same RH, starting at ∼70%, while efflorescence occurred at different humidities, i.e., at ∼35% RH for submicron particles vs. ∼50% RH for supermicron particles. This ∼15% RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5–99.4% RH range. Based on KIM, the volume-based hygroscopicity parameter, κ v , was calculated. The κ v, ws value related to the water soluble (ws) fraction was estimated to be ∼0.15 for the accumulation mode and ∼0.36 for the coarse mode, respectively. The obtained κ v, ws for the accumulation mode is in good agreement with earlier data reported for remote sites in the Amazon rain forest (κ v ≈ 0.15) and a Colorado boreal forest (κ v ≈ 0.16). We used the Zdanovskii–Stokes–Robinson (ZSR) mixing rule to predict the chemical composition dependent hygroscopicity, κ v, p . The obtained κ v, p values overestimate the experimental FDHA-KIM-derived κ v, ws by factors of 1.8 and 1.5 for the accumulation and coarse modes, respectively. This divergence can be partly explained by incomplete dissolution of the hygroscopic inorganic compounds resulting from kinetic limitations due to a sparingly soluble organic coating. The TEM and STXM-NEXAFS results indicate that aged submicron (〉300 nm) and supermicron aerosol particles possess core-shell structures with an inorganic core, and are enriched in organic carbon at the mixed particle surface. The direct FDHA kinetic studies provide a bulk diffusion coefficient of water of ∼10 −12 cm 2 s −1 indicating a semi-solid state of the organic-rich phase leading to kinetic limitations of water uptake and release during hydration and dehydration cycles. Overall the present ZOTTO data set, obtained in the growing season, has revealed a strong influence of organic carbon on the hygroscopic properties of the ambient aerosols. The sparingly soluble organic coating controls hygroscopic growth, phase transitions, and microstructural rearrangement processes. The observed kinetic limitations can strongly influence the outcome of experiments performed on multi-second time scales, such as the commonly applied HTDMA (Hygroscopicity Tandem Differential Mobility Analyzer) and CCNC (Cloud Condensation Nuclei Counter) measurements.

Description: In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical composition of aerosol particles were analyzed by X-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38% of PM in the accumulation mode and coarse mode, respectively. The water soluble fraction of organic matter was estimated to be 52 and 8% of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ∼34% in the accumulation vs. ∼47% in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5–99.4% RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same RH, starting at ∼70%, while efflorescence occurred at different humidities, i.e., at ∼35% RH for submicron particles vs. ∼50% RH for supermicron particles. This ∼15% RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5–99.4% RH range. Based on KIM, the volume-based hygroscopicity parameter, κv, was calculated. The κv, ws value related to the water soluble (ws) fraction was estimated to be ∼0.15 for the accumulation mode and ∼0.36 for the coarse mode, respectively. The obtained κv, ws for the accumulation mode is in good agreement with earlier data reported for remote sites in the Amazon rain forest (κv ≈ 0.15) and a Colorado boreal forest (κv ≈ 0.16). We used the Zdanovskii–Stokes–Robinson (ZSR) mixing rule to predict the chemical composition dependent hygroscopicity, κv, p. The obtained κv, p values overestimate the experimental FDHA-KIM-derived κv, ws by factors of 1.8 and 1.5 for the accumulation and coarse modes, respectively. This divergence can be partly explained by incomplete dissolution of the hygroscopic inorganic compounds resulting from kinetic limitations due to a sparingly soluble organic coating. The TEM and STXM-NEXAFS results indicate that aged submicron (〉300 nm) and supermicron aerosol particles possess core-shell structures with an inorganic core, and are enriched in organic carbon at the mixed particle surface. The direct FDHA kinetic studies provide a bulk diffusion coefficient of water of ∼10−12 cm2 s−1 indicating a semi-solid state of the organic-rich phase leading to kinetic limitations of water uptake and release during hydration and dehydration cycles. Overall the present ZOTTO data set, obtained in the growing season, has revealed a strong influence of organic carbon on the hygroscopic properties of the ambient aerosols. The sparingly soluble organic coating controls hygroscopic growth, phase transitions, and microstructural rearrangement processes. The observed kinetic limitations can strongly influence the outcome of experiments performed on multi-second time scales, such as the commonly applied HTDMA (Hygroscopicity Tandem Differential Mobility Analyzer) and CCNC (Cloud Condensation Nuclei Counter) measurements.

Description: In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in central Siberia (61° N, 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical compositions of aerosol particles were analyzed by x-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38 % of particulate matter (PM) in the accumulation mode and coarse mode, respectively. The water-soluble fraction of organic matter was estimated to be 52 and 8 % of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34 % in the accumulation mode vs. ~ 47 % in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5–99.4 % RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same relative humidity (RH), starting at ~ 70 %, while efflorescence occurred at different humidities, i.e., at ~ 35 % RH for submicron particles vs. ~ 50 % RH for supermicron particles. This ~ 15 % RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5–99.4 % RH range. Based on KIM, the volume-based hygroscopicity parameter, κv, was calculated. The κv,ws value related to the water-soluble (ws) fraction was estimated to be ~ 0.15 for the accumulation mode and ~ 0.36 for the coarse mode, respectively. The obtained κv,ws for the accumulation mode is in good agreement with earlier data reported for remote sites in the Amazon rain forest (κv ≈ 0.15) and a Colorado mountain forest (κv ≈ 0.16 ). We used the Zdanovskii–Stokes–Robinson (ZSR) mixing rule to predict the chemical composition dependent hygroscopicity, κv,p. The obtained κv,p values overestimate the experimental FDHA-KIM-derived κv,ws by factors of 1.8 and 1.5 for the accumulation and coarse modes, respectively. This divergence can be explained by incomplete dissolution of the hygroscopic inorganic compounds resulting from kinetic limitations due to a sparingly soluble organic coating. The TEM and STXM-NEXAFS results indicate that aged submicron (〉 300 nm) and supermicron aerosol particles possess core–shell structures with an inorganic core, and are enriched in organic carbon at the mixed particle surface. The direct FDHA kinetic studies provide a bulk diffusion coefficient of water of ~ 10−12 cm2 s−1 indicating a semi-solid state of the organic-rich phase leading to kinetic limitations of water uptake and release during hydration and dehydration cycles. Overall, the present ZOTTO data set, obtained in the growing season, has revealed a strong influence of organic carbon on the hygroscopic properties of the ambient aerosols. The sparingly soluble organic coating controls hygroscopic growth, phase transitions, and microstructural rearrangement processes. The observed kinetic limitations can strongly influence the outcome of experiments performed on multi-second timescales, such as the commonly applied HTDMA (Hygroscopicity Tandem Differential Mobility Analyzer) and CCNC (Cloud Condensation Nuclei Counter) measurements.

Description: In the framework of the European Project STAR the Mobile Aerosol Raman Lidar (MARL) of the Alfred Wegener Institute (AWI) was operated in Paramaribo, Suriname (5.8°N, 55.2°W), and carried out extensive observations of tropical cirrus clouds during the local dry season from 28 September 2004 to 16 November 2004. The coverage with ice clouds was very high with 81% in the upper troposphere (above 12 km). The frequency of occurrence of subvisual clouds was found to be clearly enhanced compared to similar observations performed with the same instrument at a station in the midlatitudes. The extinction-to-backscatter ratio of thin tropical cirrus is with 26 ± 7 sr significantly higher than that of midlatitude cirrus (16 ± 9 sr). Subvisual cirrus clouds often occur in the tropical tropopause layer (TTL) above an upper tropospheric inversion. Our observations show that the ice-forming ability of the TTL is very high. The transport of air in this layer was investigated by means of a newly developed trajectory model. We found that the occurrence of clouds is highly correlated with the temperature and humidity history of the corresponding air parcel. Air that experienced a temperature minimum before the measurement took place was generally cloud free, while air that was at its temperature minimum during the observation and thus was saturated contained ice. We also detected extremely thin cloud layers slightly above the temperature minimum in subsaturated air. The solid particles of such clouds are likely to consist of nitric acid trihydrate (NAT) rather than ice.

Description: The purpose of this study is to investigate horizontal transport processes in the winter stratosphere using data with a resolution relevant for chemistry and climate modeling. For this reason the Freie Universität Berlin Climate Middle Atmosphere Model (FUB-CMAM) with its model top at 83 km altitude, increased horizontal resolution T42 and the semi-Lagrangian transport scheme for advecting passive tracers is used. A new approach of this paper is the classification of specific transport phenomena within the stratosphere into tropical-subtropical streamers (e.g. Offermann et al., 1999) and polar vortex extrusions hereafter called polar vortex streamers. To investigate the role played by these large-scale structures on the inter-annual and seasonal variability of transport processes in northern mid-latitudes, the global occurrence of such streamers was calculated based on a 10-year model climatology, concentrating on the existence of the Arctic polar vortex. For the identification and counting of streamers, the new method of zonal anomaly was chosen. The analysis of the months October-May yielded a maximum occurrence of tropical-subtropical streamers during Arctic winter and spring in the middle and upper stratosphere. Synoptic maps revealed highest intensities in the subtropics over East Asia with a secondary maximum over the Atlantic in the northern hemisphere. Furthermore, tropical-subtropical streamers exhibited a higher occurrence than polar vortex streamers, indicating that the subtropical barrier is more permeable than the polar vortex barrier (edge) in the model, which is in good correspondence with observations (e.g. Plumb, 2002; Neu et al., 2003). Interesting for the total ozone decrease in mid-latitudes is the consideration of the lower stratosphere for tropical-subtropical streamers and the stratosphere above ~20 km altitude for polar vortex streamers, where strongest ozone depletion is observed at polar latitudes (WMO, 2003). In the lower stratosphere the FUB-CMAM simulated a climatological maximum of 10% occurrence of tropical-subtropical streamers over East-Asia/West Pacific and the Atlantic during early- and mid-winter. The results of this paper demonstrate that stratospheric streamers e.g. large-scale, tongue-like structures transporting tropical-subtropical and polar vortex air masses into mid-latitudes occur frequently during Arctic winter. They can therefore play a significant role on the strength and variability of the observed total ozone decrease at mid-latitudes and should not be neglected in future climate change studies.

Description: The purpose of this study is to investigate horizontal transport processes in the winter stratosphere using data with a high spatial and temporal resolution. For this reason the Freie Universität Berlin Climate Middle Atmosphere Model (FUB-CMAM) with its model top at 83 km altitude, increased horizontal resolution T42 and the semi-Lagrangian transport scheme for advecting passive tracers is used. A new result of this paper is the classification of specific transport phenomena within the stratosphere into tropical-subtropical streamer (e.g. Offermann et al., 1999) and polar vortex extrusions hereafter called polar vortex streamers. To investigate the role played by these large-scale structures on the inter-annual and seasonal variability of the observed negative ozone trend in northern mid-latitudes, the global occurrence of such streamers were calculated based on a 10-year model climatology, concentrating on the existence of the Arctic polar vortex. For the identification and counting of streamers, the new method of zonal anomaly was chosen, which in comparison to other methods produced the best result in this study. The analysis of the months October–May yielded a maximum occurrence of tropical-subtropical streamers during Arctic winter and spring in the middle and upper stratosphere. Synoptic maps revealed highest intensities in the subtropics over East Asia with a secondary maximum over the Atlantic in the northern hemisphere. Furthermore, tropical-subtropical streamers exhibited about a four times higher occurrence than polar vortex streamers, indicating that the subtropical barrier is more permeable than the polar vortex barrier (edge) in the model, which is in good correspondence with observations (e.g. Plumb, 2002; Neu et al., 2003). Interesting for the total ozone loss in mid-latitudes is the consideration of the lower stratosphere, where strongest ozone depletion is observed at polar latitudes (WMO, 2003). In this particular region the FUB-CMAM simulated a climatological maximum of 10% occurrence of tropical-subtropical streamers over East-Asia/West Pacific and the Atlantic during early- and mid-winter. The results of this paper demonstrate that the regular occurrence of stratospheric streamers e.g., large-scale mixing processes of tropical-subtropical and polar vortex air masses into mid-latitudes, could play a significant role on the strength and variability of the observed total ozone decrease at mid-latitudes and should not be neglected in future climate change studies.

Description: Simplified representations of spatially inhomogeneous (three-dimensional (3-D)) clouds in radiative transfer models provide systematic errors when calculating solar broadband radiative fluxes. An example is the neglect of horizontal photon transports as it is the case for the independent column approximation (ICA). The present work tries to quantify and interpret these errors on the basis of a large set of 3-D mixed phase cloud scenarios with 3-D varying extinction coefficients, scattering phase functions, and single-scattering albedos. The cloud cases result from a mesoscale atmospheric circulation model with detailed cloud microphysics. Domain-averaged cloud radiative fluxes are calculated by means of a Monte Carlo radiative transfer model. Depending on cloud type and solar zenith angle (SZA) the differences between 3-D and ICA results range from +20 W m−2 to −30 W m−2 for the upward reflected fluxes and from +10 W m−2 to −7 W m−2 for the absorbed fluxes. The mean (averaged over all cloud realizations) errors of the ICA-based upward fluxes vary between 5 W m−2 overestimation at 15°SZA and 6 W m−2 underestimation at 75°SZA. The ICA underestimates the absorbed flux by ∼1–2 W m−2 for most SZA except for 75°. It is found that neglecting the horizontal variability of the absorption and scattering properties of the cloud hydrometeors leads to a general underestimation of solar broadband absorption by as much as 15 W m−2 with average values between 4 W m−2 at small SZA and 1 W m−2 at large SZA.

Description: Submarine groundwater discharge (SGD) into coastal areas is a common global phenomenon and is rapidly gaining scientific interest due to its influence on marine ecology, the coastal sedimentary environment and its potential as a future freshwater resource. We conducted an integrated study of hydroacoustic surveys combined with geochemical porewater and water column investigations at a well‐known groundwater seep site in Eckernförde Bay (Germany). We aim to better constrain the effects of shallow gas and SGD on high frequency multibeam backscatter data and to present acoustic indications for submarine groundwater discharge. Our high‐quality hydroacoustic data reveal hitherto unknown internal structures within the pockmarks in Eckernförde Bay. Using precisely positioned sediment core samples, our hydroacoustic‐geochemical approach can differentiate intra‐pockmark regimes that were formerly assigned to pockmarks of a different nature. We demonstrate that high‐frequency multibeam data, in particular the backscatter signals, can be used to detect shallow free gas in areas of enhanced groundwater advection in muddy sediments. Intriguingly, our data reveal relatively small (typically 〈15 m across) pockmarks within the much larger, previously mapped, pockmarks. The small pockmarks, which we refer to as “intra‐pockmarks”, have formed due to the localized ascent of gas and groundwater; they manifest themselves as a new type of ‘eyed’ pockmarks, revealed by their acoustic backscatter pattern. Our data suggest that, in organic‐rich muddy sediments, morphological lows combined with a strong multibeam backscatter signal can be indicative of free shallow gas and subsequent advective groundwater flow.

Description: Corrigendum to "Dimethylsulphide (DMS) emissionsfrom the West Pacific Ocean: a potential marine source for stratospheric sulphur?" published in Atmos. Chem. Phys., 13, 8427–8437, 2013 Atmospheric Chemistry and Physics, 13, 8813-8814, 2013 Author(s): C. A. Marandino, S. Tegtmeier, K. Krüger, C. Zindler, E. L. Atlas, F. Moore, and H. W. Bange No abstract available.

Description: The Los Chocoyos (14.6°N, 91.2°W) supereruption happened ∼75,000 years ago in Guatemala and was one of the largest eruptions of the past 100,000 years. It emitted enormous amounts of sulfur, chlorine, and bromine, with multi‐decadal consequences for the global climate and environment. Here, we simulate the impact of a Los Chocoyos‐like eruption on the quasi‐biennial oscillation (QBO), an oscillation of zonal winds in the tropical stratosphere, with a comprehensive aerosol chemistry Earth System Model. We find a ∼10‐year disruption of the QBO starting 4 months post eruption, with anomalous easterly winds lasting ∼5 years, followed by westerlies, before returning to QBO conditions with a slightly prolonged periodicity. Volcanic aerosol heating and ozone depletion cooling leads to the QBO disruption and anomalous wind regimes through radiative changes and wave‐mean flow interactions. Different model ensembles, volcanic forcing scenarios and results of a second model back up the robustness of our results.

Description: We show that inflows of oxygenated waters into sulfidic layers have a strong impact on biogeochemical transformation at oxic/anoxic transition zones. Taking the pelagic methane dynamics in the Gotland Basin as an example, we performed our studies when one of the largest inflows ever recorded entered the Baltic Sea in March 2015. An inflowing gravity current transported oxic waters into the sulfidic deep layers and freshly generated a near-bottom secondary redox interface. At the upper slope, where the inflowing water masses were vigorously turbulent and the main and secondary redox interfaces in close contact to each other, methane oxidation rates inside the transition zone were found to be higher compared to the weakly turbulent basin interior. At the main redox interface in the basin center, lateral intrusions of oxygenated waters into intermediate water depth may have stimulated the growth of the methanotrophic community and their activity.

Description: Dimethylsulphide (DMS) emissions from the West Pacific Ocean: a potential marine source for the stratospheric sulphur layer Atmospheric Chemistry and Physics Discussions, 12, 30543-30570, 2012 Author(s): C. A. Marandino, S. Tegtmeier, K. Krüger, C. Zindler, E. L. Atlas, F. Moore, and H. W. Bange Sea surface and atmospheric measurements of dimethylsulphide (DMS) were performed during the TransBrom cruise in the West Pacific Ocean between Japan and Australia in October 2009. Air-sea DMS fluxes were computed between 0 and 30 μmol m −2 d −1 , which are in agreement with those computed by the current climatology, and peak emissions of marine DMS into the atmosphere were found during the occurrence of tropical storm systems. Atmospheric variability in DMS, however, did not follow that of the computed fluxes and was more related to atmospheric transport processes. The computed emissions were used as input fields for the Langrangian dispersion model FLEXPART, which was set up with actual meteorological fields from ERA-interim data and different chemical lifetimes of DMS. A comparison with aircraft in-situ data from the adjacent HIPPO2 campaign revealed an overall good agreement between modeled versus observed DMS profiles over the tropical West Pacific ocean. Based on observed DMS emissions and the meteorological fields over the cruise track region, the model projected that up to 30 g S per month in the form of DMS can be transported above 17 km in this region. This surprisingly large DMS entrainment into the stratosphere is disproportionate to the regional extent of the cruise track area and mainly due to the high convective activity in this region as simulated by the transport model. Thus, we conclude that the considerably larger area of the tropical West Pacific Ocean can be an important source of sulphur to the stratospheric persistent sulphur layer, which has not been considered as yet.

Description: Sea surface and atmospheric measurements of dimethylsulphide (DMS) were performed during the TransBrom cruise in the West Pacific Ocean between Japan and Australia in October 2009. Air-sea DMS fluxes were computed between 0 and 30 μmol m−2 d−1, which are in agreement with those computed by the current climatology, and peak emissions of marine DMS into the atmosphere were found during the occurrence of tropical storm systems. Atmospheric variability in DMS, however, did not follow that of the computed fluxes and was more related to atmospheric transport processes. The computed emissions were used as input fields for the Langrangian dispersion model FLEXPART, which was set up with actual meteorological fields from ERA-interim data and different chemical lifetimes of DMS. A comparison with aircraft in-situ data from the adjacent HIPPO2 campaign revealed an overall good agreement between modeled versus observed DMS profiles over the tropical West Pacific ocean. Based on observed DMS emissions and the meteorological fields over the cruise track region, the model projected that up to 30 g S per month in the form of DMS can be transported above 17 km in this region. This surprisingly large DMS entrainment into the stratosphere is disproportionate to the regional extent of the cruise track area and mainly due to the high convective activity in this region as simulated by the transport model. Thus, we conclude that the considerably larger area of the tropical West Pacific Ocean can be an important source of sulphur to the stratospheric persistent sulphur layer, which has not been considered as yet.

Description: Dimethylsulphide (DMS) emissions from the western Pacific Ocean: a potential marine source for stratospheric sulphur? Atmospheric Chemistry and Physics, 13, 8427-8437, 2013 Author(s): C. A. Marandino, S. Tegtmeier, K. Krüger, C. Zindler, E. L. Atlas, F. Moore, and H. W. Bange Sea surface and atmospheric measurements of dimethylsulphide (DMS) were performed during the TransBrom cruise in the western Pacific Ocean between Japan and Australia in October 2009. Air–sea DMS fluxes were computed between 0 and 30 μmol m −2 d −1 , which are in agreement with those computed by the current climatology, and peak emissions of marine DMS into the atmosphere were found during the occurrence of tropical storm systems. Atmospheric variability in DMS, however, did not follow that of the computed fluxes and was more related to atmospheric transport processes. The computed emissions were used as input fields for the Lagrangian dispersion model FLEXPART, which was set up with actual meteorological fields from ERA-Interim data and different chemical lifetimes of DMS. A comparison with aircraft in situ data from the adjacent HIPPO2 campaign revealed an overall good agreement between modelled versus observed DMS profiles over the tropical western Pacific Ocean. Based on observed DMS emissions and meteorological fields along the cruise track, the model projected that up to 30 g S per month in the form of DMS, emitted from an area of 6 × 10 4 m 2 , can be transported above 17 km. This surprisingly large DMS entrainment into the stratosphere is disproportionate to the regional extent of the area of emissions and mainly due to the high convective activity in this region as simulated by the transport model. Thus, if DMS can cross the tropical tropopause layer (TTL), we suggest that the considerably larger area of the tropical western Pacific Ocean can be a source of sulphur to the stratosphere, which has not been considered as yet.

Description: Sea surface and atmospheric measurements of dimethylsulphide (DMS) were performed during the TransBrom cruise in the western Pacific Ocean between Japan and Australia in October 2009. Air–sea DMS fluxes were computed between 0 and 30 μmol m−2 d−1, which are in agreement with those computed by the current climatology, and peak emissions of marine DMS into the atmosphere were found during the occurrence of tropical storm systems. Atmospheric variability in DMS, however, did not follow that of the computed fluxes and was more related to atmospheric transport processes. The computed emissions were used as input fields for the Lagrangian dispersion model FLEXPART, which was set up with actual meteorological fields from ERA-Interim data and different chemical lifetimes of DMS. A comparison with aircraft in situ data from the adjacent HIPPO2 campaign revealed an overall good agreement between modelled versus observed DMS profiles over the tropical western Pacific Ocean. Based on observed DMS emissions and meteorological fields along the cruise track, the model projected that up to 30 g S per month in the form of DMS, emitted from an area of 6 × 104 m2, can be transported above 17 km. This surprisingly large DMS entrainment into the stratosphere is disproportionate to the regional extent of the area of emissions and mainly due to the high convective activity in this region as simulated by the transport model. Thus, if DMS can cross the tropical tropopause layer (TTL), we suggest that the considerably larger area of the tropical western Pacific Ocean can be a source of sulphur to the stratosphere, which has not been considered as yet.

Description: Direct oceanic emissions unlikely to account for the missing source of atmospheric carbonyl sulfide Sinikka T. Lennartz, Christa A. Marandino, Marc von Hobe, Pau Cortes, Birgit Quack, Rafel Simo, Dennis Booge, Andrea Pozzer, Tobias Steinhoff, Damian L. Arevalo-Martinez, Corinna Kloss, Astrid Bracher, Rüdiger Röttgers, Elliot Atlas, and Kirstin Krüger Atmos. Chem. Phys., 17, 385-402, doi:10.5194/acp-17-385-2017, 2017 We present new sea surface and marine boundary layer measurements of carbonyl sulfide, the most abundant sulfur gas in the atmosphere, and calculate an oceanic emission estimate. Our results imply that oceanic emissions are very unlikely to account for the missing source in the atmospheric budget that is currently discussed for OCS.

Description: Direct oceanic emissions unlikely to account for the missing source of atmospheric carbonyl sulfide Sinikka T. Lennartz, Christa A. Marandino, Marc von Hobe, Pau Cortes, Birgit Quack, Rafel Simo, Dennis Booge, Andrea Pozzer, Tobias Steinhoff, Damian L. Arevalo-Martinez, Corinna Kloss, Astrid Bracher, Rüdiger Röttgers, Elliot Atlas, and Kirstin Krüger Atmos. Chem. Phys., 17, 385-402, doi:10.5194/acp-17-385-2017, 2017 We present new sea surface and marine boundary layer measurements of carbonyl sulfide, the most abundant sulfur gas in the atmosphere, and calculate an oceanic emission estimate. Our results imply that oceanic emissions are very unlikely to account for the missing source in the atmospheric budget that is currently discussed for OCS.

Description: The climate active trace-gas carbonyl sulfide (OCS) is the most abundant sulfur gas in the atmosphere. A missing source in its atmospheric budget is currently suggested, resulting from an upward revision of the vegetation sink. Tropical oceanic emissions have been proposed to close the resulting gap in the atmospheric budget. We present a bottom-up approach including (i) new observations of OCS in surface waters of the tropical Atlantic, Pacific and Indian oceans and (ii) a further improved global box model to show that direct OCS emissions are unlikely to account for the missing source. The box model suggests an undersaturation of the surface water with respect to OCS integrated over the entire tropical ocean area and, further, global annual direct emissions of OCS well below that suggested by top-down estimates. In addition, we discuss the potential of indirect emission from CS2 and dimethylsulfide (DMS) to account for the gap in the atmospheric budget. This bottom-up estimate of oceanic emissions has implications for using OCS as a proxy for global terrestrial CO2 uptake, which is currently impeded by the inadequate quantification of atmospheric OCS sources and sinks.

Description: Mesoscale eddies are frequently observed in the Eastern Tropical North Atlantic (ETNA), yet their effects on the transport and distribution of biogeochemical solutes, and specifically on the production and remineralization of dissolved organic matter (DOM) remain difficult to elucidate. Here, we investigated the submesoscale variability of chromophoric DOM (CDOM) and fluorescent DOM (FDOM) together with microbial production and remineralization processes in two cyclonic eddies (CEs) in the ETNA during summer and winter 2019. One CE, formed near the coast off Mauritania during the post-upwelling season, was sampled along a ∼900 km zonal corridor between Mauritania and the Cape Verde Islands. The other CE, formed nearby Brava Island, was out of coastal influence. Four fluorescent components were identified with parallel factor analysis, two humic-like, and two protein-like components. Humic-like FDOM components correlated to optode-based community respiration and were also good indicators of upwelling associated with the Brava Island CE as they correlated to physical parameters (e.g., temperature) and to dissolved inorganic nitrogen. The tryptophan-like FDOM components correlated with the carbon and nitrogen content of semi-labile DOM, phytoplankton biomass, community respiration, and bacterial production. Overall, our study revealed that DOM optical properties are suitable for tracing freshly produced organic matter and the transport of remineralized DOM within offshore eddies. Key Points: - Four fluorescent dissolved organic matter (FDOM) components were studied in two cyclonic eddies (CEs) in the Eastern Tropical North Atlantic - Tryptophan-like FDOM was an indicator of the CEs' productivity as it correlated with semi-labile dissolved organic matter and microbial metabolic activities - Humic-like FDOM was a by-product of microbial respiration; its distribution within an offshore CE covaried with nutrient upwelling

Description: Drivers of diel and regional variations of halocarbon emissions from the tropical North East Atlantic Atmospheric Chemistry and Physics Discussions, 13, 19701-19750, 2013 Author(s): H. Hepach, B. Quack, F. Ziska, S. Fuhlbrügge, E. L. Atlas, I. Peeken, K. Krüger, and D. W. R. Wallace Methyl iodide (CH 3 I}, bromoform (CHBr 3 ) and dibromomethane (CH 2 Br 2 ), which are produced naturally in the oceans, take part in ozone chemistry both in the troposphere and the stratosphere. The significance of oceanic upwelling regions for emissions of these trace gases in the global context is still uncertain although they have been identified as important source regions. To better quantify the role of upwelling areas in current and future climate, this paper analyzes major factors that influenced halocarbon emissions from the tropical North East Atlantic including the Mauritanian upwelling during the DRIVE expedition. Diel and regional variability of oceanic and atmospheric CH 3 I, CHBr 3 and CH 2 Br 2 was determined along with biological and meteorological parameters at six 24 h-stations. Low oceanic concentrations of CH 3I from 0.1–5.4 pmol L -1 were equally distributed throughout the investigation area. CHBr 3 of 1.0–42.4 pmol L -1 and CH 2 Br 2 of 1.0–9.4 pmol L -1 were measured with maximum concentrations close to the Mauritanian coast. Atmospheric mixing rations of CH 3 I of up to 3.3, CHBr 3 to 8.9 and CH 2 Br 2 to 3.1 ppt above the upwelling and 1.8, 12.8, respectively 2.2 ppt at a Cape Verdean coast were detected during the campaign. While diel variability in CH 3 I emissions could be mainly ascribed to oceanic non-biological production, no main driver was identified for its emissions in the entire study region. In contrast, oceanic bromocarbons resulted from biogenic sources which were identified as regional drivers of their sea-to-air fluxes. The diel impact of wind speed on bromocarbon emissions increased with decreasing distance to the coast. The height of the marine atmospheric boundary layer (MABL) was determined as an additional factor influencing halocarbon emissions. Oceanic and atmospheric halocarbons correlated well in the study region and in combination with high oceanic CH 3I , CHBr 3 and CH 2 Br 2 concentrations, local hot spots of atmospheric halocarbons could solely be explained by marine sources. This conclusion is in contrast with previous studies that hypothesized the occurrence of elevated atmospheric halocarbons over the eastern tropical Atlantic mainly originating from the West-African continent.

Description: Drivers of diel and regional variations of halocarbon emissions from the tropical North East Atlantic Atmospheric Chemistry and Physics, 14, 1255-1275, 2014 Author(s): H. Hepach, B. Quack, F. Ziska, S. Fuhlbrügge, E. L. Atlas, K. Krüger, I. Peeken, and D. W. R. Wallace Methyl iodide (CH 3 I), bromoform (CHBr 3 ) and dibromomethane (CH 2 Br 2 ), which are produced naturally in the oceans, take part in ozone chemistry both in the troposphere and the stratosphere. The significance of oceanic upwelling regions for emissions of these trace gases in the global context is still uncertain although they have been identified as important source regions. To better quantify the role of upwelling areas in current and future climate, this paper analyzes major factors that influenced halocarbon emissions from the tropical North East Atlantic including the Mauritanian upwelling during the DRIVE expedition. Diel and regional variability of oceanic and atmospheric CH 3 I, CHBr 3 and CH 2 Br 2 was determined along with biological and physical parameters at six 24 h-stations. Low oceanic concentrations of CH 3 I from 0.1–5.4 pmol L −1 were equally distributed throughout the investigation area. CHBr 3 and CH 2 Br 2 from 1.0 to 42.4 pmol L −1 and to 9.4 pmol L −1 , respectively were measured with maximum concentrations close to the Mauritanian coast. Atmospheric CH 3 I, CHBr 3 , and CH 2 Br 2 of up to 3.3, 8.9, and 3.1 ppt, respectively were detected above the upwelling, as well as up to 1.8, 12.8, and 2.2 ppt at the Cape Verdean coast. While diel variability in CH 3 I emissions could be mainly ascribed to oceanic non-biological production, no main driver was identified for its emissions over the entire study region. In contrast, biological parameters showed the greatest influence on the regional distribution of sea-to-air fluxes of bromocarbons. The diel impact of wind speed on bromocarbon emissions increased with decreasing distance to the coast. The height of the marine atmospheric boundary layer (MABL) influenced halocarbon emissions via its influence on atmospheric mixing ratios. Oceanic and atmospheric halocarbons correlated well in the study region, and in combination with high oceanic CH 3 I, CHBr 3 and CH 2 Br 2 concentrations, local hot spots of atmospheric halocarbons could solely be explained by marine sources. This conclusion is in contrast to previous studies that hypothesized elevated atmospheric halocarbons above the eastern tropical Atlantic to be mainly originated from the West-African continent.

Description: Methyl iodide (CH3I}, bromoform (CHBr3) and dibromomethane (CH2Br2), which are produced naturally in the oceans, take part in ozone chemistry both in the troposphere and the stratosphere. The significance of oceanic upwelling regions for emissions of these trace gases in the global context is still uncertain although they have been identified as important source regions. To better quantify the role of upwelling areas in current and future climate, this paper analyzes major factors that influenced halocarbon emissions from the tropical North East Atlantic including the Mauritanian upwelling during the DRIVE expedition. Diel and regional variability of oceanic and atmospheric CH3I, CHBr3 and CH2Br2 was determined along with biological and meteorological parameters at six 24 h-stations. Low oceanic concentrations of CH3I from 0.1–5.4 pmol L-1 were equally distributed throughout the investigation area. CHBr3 of 1.0–42.4 pmol L-1 and CH2Br2 of 1.0–9.4 pmol L-1 were measured with maximum concentrations close to the Mauritanian coast. Atmospheric mixing rations of CH3I of up to 3.3, CHBr3 to 8.9 and CH2Br2 to 3.1 ppt above the upwelling and 1.8, 12.8, respectively 2.2 ppt at a Cape Verdean coast were detected during the campaign. While diel variability in CH3I emissions could be mainly ascribed to oceanic non-biological production, no main driver was identified for its emissions in the entire study region. In contrast, oceanic bromocarbons resulted from biogenic sources which were identified as regional drivers of their sea-to-air fluxes. The diel impact of wind speed on bromocarbon emissions increased with decreasing distance to the coast. The height of the marine atmospheric boundary layer (MABL) was determined as an additional factor influencing halocarbon emissions. Oceanic and atmospheric halocarbons correlated well in the study region and in combination with high oceanic CH3I, CHBr3 and CH2Br2 concentrations, local hot spots of atmospheric halocarbons could solely be explained by marine sources. This conclusion is in contrast with previous studies that hypothesized the occurrence of elevated atmospheric halocarbons over the eastern tropical Atlantic mainly originating from the West-African continent.

Description: Methyl iodide (CH3I), bromoform (CHBr3) and dibromomethane (CH2Br2), which are produced naturally in the oceans, take part in ozone chemistry both in the troposphere and the stratosphere. The significance of oceanic upwelling regions for emissions of these trace gases in the global context is still uncertain although they have been identified as important source regions. To better quantify the role of upwelling areas in current and future climate, this paper analyzes major factors that influenced halocarbon emissions from the tropical North East Atlantic including the Mauritanian upwelling during the DRIVE expedition. Diel and regional variability of oceanic and atmospheric CH3I, CHBr3 and CH2Br2 was determined along with biological and physical parameters at six 24 h-stations. Low oceanic concentrations of CH3I from 0.1–5.4 pmol L−1 were equally distributed throughout the investigation area. CHBr3 and CH2Br2 from 1.0 to 42.4 pmol L−1 and to 9.4 pmol L−1, respectively were measured with maximum concentrations close to the Mauritanian coast. Atmospheric CH3I, CHBr3, and CH2Br2 of up to 3.3, 8.9, and 3.1 ppt, respectively were detected above the upwelling, as well as up to 1.8, 12.8, and 2.2 ppt at the Cape Verdean coast. While diel variability in CH3I emissions could be mainly ascribed to oceanic non-biological production, no main driver was identified for its emissions over the entire study region. In contrast, biological parameters showed the greatest influence on the regional distribution of sea-to-air fluxes of bromocarbons. The diel impact of wind speed on bromocarbon emissions increased with decreasing distance to the coast. The height of the marine atmospheric boundary layer (MABL) influenced halocarbon emissions via its influence on atmospheric mixing ratios. Oceanic and atmospheric halocarbons correlated well in the study region, and in combination with high oceanic CH3I, CHBr3 and CH2Br2 concentrations, local hot spots of atmospheric halocarbons could solely be explained by marine sources. This conclusion is in contrast to previous studies that hypothesized elevated atmospheric halocarbons above the eastern tropical Atlantic to be mainly originated from the West-African continent.

Description: Emission and transport of bromocarbons: from the West Pacific ocean into the stratosphere Atmospheric Chemistry and Physics, 12, 10633-10648, 2012 Author(s): S. Tegtmeier, K. Krüger, B. Quack, E. L. Atlas, I. Pisso, A. Stohl, and X. Yang Oceanic emissions of halogenated very short-lived substances (VSLS) are expected to contribute significantly to the stratospheric halogen loading and therefore to ozone depletion. The amount of VSLS transported into the stratosphere is estimated based on in-situ observations around the tropical tropopause layer (TTL) and on modeling studies which mostly use prescribed global emission scenarios to reproduce observed atmospheric concentrations. In addition to upper-air VSLS measurements, direct observations of oceanic VSLS emissions are available along ship cruise tracks. Here we use such in-situ observations of VSLS emissions from the West Pacific and tropical Atlantic together with an atmospheric Lagrangian transport model to estimate the direct contribution of bromoform (CHBr 3 ), and dibromomethane (CH 2 Br 2 ) to the stratospheric bromine loading as well as their ozone depletion potential. Our emission-based estimates of VSLS profiles are compared to upper-air observations and thus link observed oceanic emissions and in situ TTL measurements. This comparison determines how VSLS emissions and transport in the cruise track regions contribute to global upper-air VSLS estimates. The West Pacific emission-based profiles and the global upper-air observations of CHBr 3 show a relatively good agreement indicating that emissions from the West Pacific provide an average contribution to the global CHBr 3 budget. The tropical Atlantic, although also being a CHBr 3 source region, is of less importance for global upper-air CHBr 3 estimates as revealed by the small emission-based abundances in the TTL. Western Pacific CH 2 Br 2 emission-based estimates are considerably smaller than upper-air observations as a result of the relatively low sea-to-air flux found in the West Pacific. Together, CHBr 3 and CH 2 Br 2 emissions from the West Pacific are projected to contribute to the stratospheric bromine budget with 0.4 pptv Br on average and 2.3 pptv Br for cases of maximum emissions through product and source gas injection. These relatively low estimates reveal that the tropical West Pacific, although characterized by strong convective transport, might overall contribute less VSLS to the stratospheric bromine budget than other regions as a result of only low CH 2 Br 2 and moderate CHBr 3 oceanic emissions.

Description: Oceanic emissions of halogenated very short-lived substances (VSLS) are expected to contribute significantly to the stratospheric halogen loading and therefore to ozone depletion. The amount of VSLS transported into the stratosphere is estimated based on in-situ observations around the tropical tropopause layer (TTL) and on modeling studies which mostly use prescribed global emission scenarios to reproduce observed atmospheric concentrations. In addition to upper-air VSLS measurements, direct observations of oceanic VSLS emissions are available along ship cruise tracks. Here we use such in-situ observations of VSLS emissions from the West Pacific and tropical Atlantic together with an atmospheric Lagrangian transport model to estimate the direct contribution of bromoform (CHBr3), and dibromomethane (CH2Br2) to the stratospheric bromine loading as well as their ozone depletion potential. Our emission-based estimates of VSLS profiles are compared to upper-air observations and thus link observed oceanic emissions and in situ TTL measurements. This comparison determines how VSLS emissions and transport in the cruise track regions contribute to global upper-air VSLS estimates. The West Pacific emission-based profiles and the global upper-air observations of CHBr3 show a relatively good agreement indicating that emissions from the West Pacific provide an average contribution to the global CHBr3 budget. The tropical Atlantic, although also being a CHBr3 source region, is of less importance for global upper-air CHBr3 estimates as revealed by the small emission-based abundances in the TTL. Western Pacific CH2Br2 emission-based estimates are considerably smaller than upper-air observations as a result of the relatively low sea-to-air flux found in the West Pacific. Together, CHBr3 and CH2Br2 emissions from the West Pacific are projected to contribute to the stratospheric bromine budget with 0.4 pptv Br on average and 2.3 pptv Br for cases of maximum emissions through product and source gas injection. These relatively low estimates reveal that the tropical West Pacific, although characterized by strong convective transport, might overall contribute less VSLS to the stratospheric bromine budget than other regions as a result of only low CH2Br2 and moderate CHBr3 oceanic emissions.

Description: The science guiding the EUREC4A campaign and its measurements is presented. EUREC4A comprised roughly 5 weeks of measurements in the downstream winter trades of the North Atlantic – eastward and southeastward of Barbados. Through its ability to characterize processes operating across a wide range of scales, EUREC4A marked a turning point in our ability to observationally study factors influencing clouds in the trades, how they will respond to warming, and their link to other components of the earth system, such as upper-ocean processes or the life cycle of particulate matter. This characterization was made possible by thousands (2500) of sondes distributed to measure circulations on meso- (200 km) and larger (500 km) scales, roughly 400 h of flight time by four heavily instrumented research aircraft; four global-class research vessels; an advanced ground-based cloud observatory; scores of autonomous observing platforms operating in the upper ocean (nearly 10 000 profiles), lower atmosphere (continuous profiling), and along the air–sea interface; a network of water stable isotopologue measurements; targeted tasking of satellite remote sensing; and modeling with a new generation of weather and climate models. In addition to providing an outline of the novel measurements and their composition into a unified and coordinated campaign, the six distinct scientific facets that EUREC4A explored – from North Brazil Current rings to turbulence-induced clustering of cloud droplets and its influence on warm-rain formation – are presented along with an overview of EUREC4A's outreach activities, environmental impact, and guidelines for scientific practice. Track data for all platforms are standardized and accessible at https://doi.org/10.25326/165 (Stevens, 2021), and a film documenting the campaign is provided as a video supplement.

Description: This study performed the first assessment of the volcanic gas output from the Central Volcanic Zone (CVZ) of northern Chile. We present the fluxes and compositions of volcanic gases (H2O, CO2, H2, HCl, HF, and HBr) from five of the most actively degassing volcanoes in this region—Láscar, Lastarria, Putana, Ollagüe, and San Pedro—obtained during field campaigns in 2012 and 2013. The inferred gas plume compositions for Láscar and Lastarria (CO2/Stot = 0.9–2.2; Stot/HCl = 1.4–3.4) are similar to those obtained in the Southern Volcanic Zone of Chile, suggesting uniform magmatic gas fingerprint throughout the Chilean arc. Combining these compositions with our own UV spectroscopy measurements of the SO2 output (summing to ~1800 t d−1 for the CVZ), we calculate a cumulative CO2 output of 1743–1988 t d−1 and a total volatiles output of 〉20,200 t d−1.

Description: Acetone is one of the most abundant oxygenated volatile organic compounds (VOCs) in the atmosphere. The oceans impose a strong control on atmospheric acetone, yet the oceanic fluxes of acetone remain poorly constrained. In this work, the global budget of acetone is evaluated using two global models: CAM‐chem and GEOS‐Chem. CAM‐chem uses an online air‐sea exchange framework to calculate the bidirectional oceanic acetone fluxes, which is coupled to a data‐oriented machine‐learning approach. The machine‐learning algorithm is trained using a global suite of seawater acetone measurements. GEOS‐Chem uses a fixed surface seawater concentration of acetone to calculate the oceanic fluxes. Both model simulations are compared to airborne observations from a recent global‐scale, multiseasonal campaign, the NASA Atmospheric Tomography Mission (ATom). We find that both CAM‐chem and GEOS‐Chem capture the measured acetone vertical distributions in the remote atmosphere reasonably well. The combined observational and modeling analysis suggests that (i) the ocean strongly regulates the atmospheric budget of acetone. The tropical and subtropical oceans are mostly a net source of acetone, while the high‐latitude oceans are a net sink. (ii) CMIP6 anthropogenic emission inventory may underestimate acetone and/or its precursors in the Northern Hemisphere. (iii) The MEGAN biogenic emissions model may overestimate acetone and/or its precursors, and/or the biogenic oxidation mechanisms may overestimate the acetone yields. (iv) The models consistently overestimate acetone in the upper troposphere‐lower stratosphere over the Southern Ocean in austral winter. (v) Acetone contributes up to 30–40% of hydroxyl radical production in the tropical upper troposphere/lower stratosphere.

Description: Global sea-to-air flux climatology for bromoform, dibromomethane and methyl iodide Atmospheric Chemistry and Physics Discussions, 13, 5601-5648, 2013 Author(s): F. Ziska, B. Quack, K. Abrahamsson, S. D. Archer, E. Atlas, T. Bell, J. H. Butler, L. J. Carpenter, C. E. Jones, N. R. P. Harris, H. Hepach, K. G. Heumann, C. Hughes, J. Kuss, K. Krüger, P. Liss, R. M. Moore, A. Orlikowska, S. Raimund, C. E. Reeves, W. Reifenhäuser, A. D. Robinson, C. Schall, T. Tanhua, S. Tegtmeier, S. Turner, L. Wang, D. Wallace, J. Williams, H. Yamamoto, S. Yvon-Lewis, and Y. Yokouchi Volatile halogenated organic compounds containing bromine and iodine, which are naturally produced in the ocean, are involved in ozone depletion in both the troposphere and stratosphere. Three prominent compounds transporting large amounts of marine halogens into the atmosphere are bromoform (CHBr 3 ), dibromomethane (CH 2 Br 2 ) and methyl iodide (CH 3 I). The input of marine halogens to the stratosphere is based on observations and modeling studies using low resolution oceanic emission scenarios derived from top down approaches. In order to improve emission inventory estimates, we calculate data-based high resolution global sea-to-air flux estimates of these compounds from surface observations within the HalOcAt database ( https://halocat.geomar.de/ ). Global maps of marine and atmospheric surface concentrations are derived from the data which are divided into coastal, shelf and open ocean regions. Considering physical and biogeochemical characteristics of ocean and atmosphere, the open ocean water and atmosphere data are classified into 21 regions. The available data are interpolated onto a 1° × 1° grid while missing grid values are interpolated with latitudinal and longitudinal dependent regression techniques reflecting the compounds' distributions. With the generated surface concentration climatologies for the ocean and atmosphere, global concentration gradients and sea-to-air fluxes are calculated. Based on these calculations we estimate a total global flux of 1.5/2.5 Gmol Br yr −1 for CHBr 3 , 0.78/0.98 Gmol Br yr −1 for CH 2 Br 2 and 1.24/1.45 Gmol I yr −1 for CH 3 I (Robust Fit/Ordinary Least Square regression technique). Contrary to recent studies, negative fluxes occur in each sea-to-air flux climatology, mainly in the Arctic and Antarctic region. "Hot spots" for global polybromomethane emissions are located in the equatorial region, whereas methyl iodide emissions are enhanced in the subtropical gyre regions. Inter-annual and seasonal variation is contained within our calculations for all three compounds. Compared to earlier studies, our global fluxes are at the lower end of estimates, especially for bromoform. An underrepresentation of coastal emissions and of extreme events in our estimate might explain the mismatch between our bottom up emission estimate and top down approaches.

Description: Global sea-to-air flux climatology for bromoform, dibromomethane and methyl iodide Atmospheric Chemistry and Physics, 13, 8915-8934, 2013 Author(s): F. Ziska, B. Quack, K. Abrahamsson, S. D. Archer, E. Atlas, T. Bell, J. H. Butler, L. J. Carpenter, C. E. Jones, N. R. P. Harris, H. Hepach, K. G. Heumann, C. Hughes, J. Kuss, K. Krüger, P. Liss, R. M. Moore, A. Orlikowska, S. Raimund, C. E. Reeves, W. Reifenhäuser, A. D. Robinson, C. Schall, T. Tanhua, S. Tegtmeier, S. Turner, L. Wang, D. Wallace, J. Williams, H. Yamamoto, S. Yvon-Lewis, and Y. Yokouchi Volatile halogenated organic compounds containing bromine and iodine, which are naturally produced in the ocean, are involved in ozone depletion in both the troposphere and stratosphere. Three prominent compounds transporting large amounts of marine halogens into the atmosphere are bromoform (CHBr 3 ), dibromomethane (CH 2 Br 2 ) and methyl iodide (CH 3 I). The input of marine halogens to the stratosphere has been estimated from observations and modelling studies using low-resolution oceanic emission scenarios derived from top-down approaches. In order to improve emission inventory estimates, we calculate data-based high resolution global sea-to-air flux estimates of these compounds from surface observations within the HalOcAt (Halocarbons in the Ocean and Atmosphere) database ( https://halocat.geomar.de/ ). Global maps of marine and atmospheric surface concentrations are derived from the data which are divided into coastal, shelf and open ocean regions. Considering physical and biogeochemical characteristics of ocean and atmosphere, the open ocean water and atmosphere data are classified into 21 regions. The available data are interpolated onto a 1°×1° grid while missing grid values are interpolated with latitudinal and longitudinal dependent regression techniques reflecting the compounds' distributions. With the generated surface concentration climatologies for the ocean and atmosphere, global sea-to-air concentration gradients and sea-to-air fluxes are calculated. Based on these calculations we estimate a total global flux of 1.5/2.5 Gmol Br yr −1 for CHBr 3 , 0.78/0.98 Gmol Br yr −1 for CH 2 Br 2 and 1.24/1.45 Gmol Br yr −1 for CH 3 I (robust fit/ordinary least squares regression techniques). Contrary to recent studies, negative fluxes occur in each sea-to-air flux climatology, mainly in the Arctic and Antarctic regions. "Hot spots" for global polybromomethane emissions are located in the equatorial region, whereas methyl iodide emissions are enhanced in the subtropical gyre regions. Inter-annual and seasonal variation is contained within our flux calculations for all three compounds. Compared to earlier studies, our global fluxes are at the lower end of estimates, especially for bromoform. An under-representation of coastal emissions and of extreme events in our estimate might explain the mismatch between our bottom-up emission estimate and top-down approaches.

Description: Volatile halogenated organic compounds containing bromine and iodine, which are naturally produced in the ocean, are involved in ozone depletion in both the troposphere and stratosphere. Three prominent compounds transporting large amounts of marine halogens into the atmosphere are bromoform (CHBr3), dibromomethane (CH2Br2) and methyl iodide (CH3I). The input of marine halogens to the stratosphere has been estimated from observations and modelling studies using low-resolution oceanic emission scenarios derived from top-down approaches. In order to improve emission inventory estimates, we calculate data-based high resolution global sea-to-air flux estimates of these compounds from surface observations within the HalOcAt (Halocarbons in the Ocean and Atmosphere) database (https://halocat.geomar.de/). Global maps of marine and atmospheric surface concentrations are derived from the data which are divided into coastal, shelf and open ocean regions. Considering physical and biogeochemical characteristics of ocean and atmosphere, the open ocean water and atmosphere data are classified into 21 regions. The available data are interpolated onto a 1°×1° grid while missing grid values are interpolated with latitudinal and longitudinal dependent regression techniques reflecting the compounds' distributions. With the generated surface concentration climatologies for the ocean and atmosphere, global sea-to-air concentration gradients and sea-to-air fluxes are calculated. Based on these calculations we estimate a total global flux of 1.5/2.5 Gmol Br yr−1 for CHBr3, 0.78/0.98 Gmol Br yr−1 for CH2Br2 and 1.24/1.45 Gmol Br yr−1 for CH3I (robust fit/ordinary least squares regression techniques). Contrary to recent studies, negative fluxes occur in each sea-to-air flux climatology, mainly in the Arctic and Antarctic regions. "Hot spots" for global polybromomethane emissions are located in the equatorial region, whereas methyl iodide emissions are enhanced in the subtropical gyre regions. Inter-annual and seasonal variation is contained within our flux calculations for all three compounds. Compared to earlier studies, our global fluxes are at the lower end of estimates, especially for bromoform. An under-representation of coastal emissions and of extreme events in our estimate might explain the mismatch between our bottom-up emission estimate and top-down approaches.

Description: Volatile halogenated organic compounds containing bromine and iodine, which are naturally produced in the ocean, are involved in ozone depletion in both the troposphere and stratosphere. Three prominent compounds transporting large amounts of marine halogens into the atmosphere are bromoform (CHBr3), dibromomethane (CH2Br2) and methyl iodide (CH3I). The input of marine halogens to the stratosphere is based on observations and modeling studies using low resolution oceanic emission scenarios derived from top down approaches. In order to improve emission inventory estimates, we calculate data-based high resolution global sea-to-air flux estimates of these compounds from surface observations within the HalOcAt database (https://halocat.geomar.de/). Global maps of marine and atmospheric surface concentrations are derived from the data which are divided into coastal, shelf and open ocean regions. Considering physical and biogeochemical characteristics of ocean and atmosphere, the open ocean water and atmosphere data are classified into 21 regions. The available data are interpolated onto a 1° × 1° grid while missing grid values are interpolated with latitudinal and longitudinal dependent regression techniques reflecting the compounds' distributions. With the generated surface concentration climatologies for the ocean and atmosphere, global concentration gradients and sea-to-air fluxes are calculated. Based on these calculations we estimate a total global flux of 1.5/2.5 Gmol Br yr−1 for CHBr3, 0.78/0.98 Gmol Br yr−1 for CH2Br2 and 1.24/1.45 Gmol I yr−1 for CH3I (Robust Fit/Ordinary Least Square regression technique). Contrary to recent studies, negative fluxes occur in each sea-to-air flux climatology, mainly in the Arctic and Antarctic region. "Hot spots" for global polybromomethane emissions are located in the equatorial region, whereas methyl iodide emissions are enhanced in the subtropical gyre regions. Inter-annual and seasonal variation is contained within our calculations for all three compounds. Compared to earlier studies, our global fluxes are at the lower end of estimates, especially for bromoform. An underrepresentation of coastal emissions and of extreme events in our estimate might explain the mismatch between our bottom up emission estimate and top down approaches.

Description: Arctic river deltas and deltaic near-shore zones represent important land–ocean transition zones influencing sediment dynamics and nutrient fluxes from permafrost-affected terrestrial ecosystems into the coastal Arctic Ocean. To accurately model fluvial carbon and freshwater export from rapidly changing river catchments as well as assess impacts of future change on the Arctic shelf and coastal ecosystems, we need to understand the sea floor characteristics and topographic variety of the coastal zones. To date, digital bathymetrical data from the poorly accessible, shallow, and large areas of the eastern Siberian Arctic shelves are sparse. We have digitized bathymetrical information for nearly 75 000 locations from large-scale (1:25 000–1:500 000) current and historical nautical maps of the Lena Delta and the Kolyma Gulf region in northeastern Siberia. We present the first detailed and seamless digital models of coastal zone bathymetry for both delta and gulf regions in 50 and 200 m spatial resolution. We validated the resulting bathymetry layers using a combination of our own water depth measurements and a collection of available depth measurements, which showed a strong correlation (r〉0.9). Our bathymetrical models will serve as an input for a high-resolution coupled hydrodynamic–ecosystem model to better quantify fluvial and coastal carbon fluxes to the Arctic Ocean, but they may be useful for a range of other studies related to Arctic delta and near-shore dynamics such as modeling of submarine permafrost, near-shore sea ice, or shelf sediment transport. The new digital high-resolution bathymetry products are available on the PANGAEA data set repository for the Lena Delta (https://doi.org/10.1594/PANGAEA.934045; Fuchs et al., 2021a) and Kolyma Gulf region (https://doi.org/10.1594/PANGAEA.934049; Fuchs et al., 2021b), respectively. Likewise, the depth validation data are available on PANGAEA as well (https://doi.org/10.1594/PANGAEA.933187; Fuchs et al., 2021c).

Description: “Flip‐flop” detachment mode represents an endmember type of lithosphere‐scale faulting observed at almost amagmatic sections of ultraslow‐spreading mid‐ocean ridges. Recent numerical experiments using an imposed steady temperature structure show that an axial temperature maximum is essential to trigger flip‐flop faults by focusing flexural strain in the footwall of the active fault. However, ridge segments without significant melt budget are more likely to be in a transient thermal state controlled, at least partly, by the faulting dynamics themselves. Therefore, we investigate which processes control the thermal structure of the lithosphere and how feedbacks with the deformation mechanisms can explain observed faulting patterns. We present results of 2‐D thermo‐mechanical numerical modeling including serpentinization reactions and dynamic grain size evolution. The model features a novel form of parametrized hydrothermal cooling along fault zones as well as the thermal and rheological effects of periodic sill intrusions. We find that the interplay of hydrothermal fault zone cooling and periodic sill intrusions in the footwall facilitates the flip‐flop detachment mode. Hydrothermal cooling of the fault zone pushes the temperature maximum into the footwall, while intrusions near the temperature maximum further weaken the rock and promote the formation of new faults with opposite polarity. Our model allows us to put constraints on the magnitude of two processes, and we obtain most reasonable melt budgets and hydrothermal heat fluxes if both are considered. Furthermore, we frequently observe two other faulting modes in our experiments complementing flip‐flop faulting to yield a potentially more robust alternative interpretation for existing observations. Plain Language Summary At mid‐ocean ridges, two plates diverge and new seafloor is created. The nature and appearance of this new seafloor strongly depend on spreading velocity and the availability of magmatic melts. At one of the melt‐poorest and slowest‐spreading ridges, a special form of large‐scale tectonic faults, so‐called flip‐flop detachments, can be observed. Tectonic faults can act as pathways for fluids circulating through the seafloor, which provides a significant cooling effect for the young plate. The interplay of magmatic activity, faulting and fluid circulation is evident at many different ridges with different magmatic activity and spreading rates. Flip‐flop faulting is restricted to only a few ridge sections worldwide, and we here investigate the prerequisites for this special spreading mode. To do so, we set up a computer model of an ultraslow‐spreading mid‐ocean ridge including the effects of sparse magmatism as well as the cooling effect associated with fluid circulation. We find that feedbacks between faulting dynamics, hydrothermal cooling and magmatic activity control the magnitude and spatial location of each individual process. Seafloor and subsurface observations are best explained by calculations with moderate melt input and hydrothermal circulation acting together. Key Points We implemented hydrothermal cooling and magmatic intrusion in a thermo‐mechanical model to explain detachment faulting at ultraslow ridges Stable flip‐flop detachment faulting is observed for setups considering both melt input and hydrothermal heat fluxes at realistic magnitudes Two other faulting modes frequently observed in our model offer potential alternative interpretations for existing seafloor observations

Description: An array of broadband seismometers transecting the Talamanca Range in southern Costa Rica was operated from 2005 until 2007. In combination with data from a short‐period network near Quepos in central Costa Rica, this data is analyzed by the receiver function method to image the crustal structure in south‐central Costa Rica. Two strong positive signals are seen in the migrated images, interpreted as the Moho (at around 35 km depth) and an intra‐crustal discontinuity (15 km depth). A relatively flat crustal and Moho interface underneath the north‐east flank of the Talamanca Range can be followed for a lateral distance of about 50 km parallel to the trench, with only slight changes in the overall geometry. Closer to the coast, the topography of the discontinuities shows several features, most notably a deeper Moho underneath the Talamanca Mountain Range and volcanic arc. Under the highest part of the mountain ranges, the Moho reaches a depth of about 50 km, which indicates that the mountain ranges are approximately isostatically compensated. Local deviations from the crustal thickness expected for isostatic equilibrium occur under the active volcanic arc and in south Costa Rica. In the transition region between the active volcanic arc and the Talamanca Range, both the Moho and intracrustal discontinuity appear distorted, possibly related to the southern edge of the active volcanic zone and deformation within the southern part of the Central Costa Rica Deformed Belt. Near the volcanoes Irazu and Turrialba, a shallow converter occurs, correlating with a low‐velocity, low‐density body seen in tomography and gravimetry. Applying a grid search for the crustal interface depth and vp/vs ratio cannot constrain vp/vs values well, but points to generally low values (〈1.7) in the upper crust. This is consistent with quartz‐rich rocks forming the mountain range.

Description: Forecasting and early warning systems are important investments to protect lives, properties and livelihood. While early warning systems are frequently used to predict the magnitude, location and timing of potentially damaging events, these systems rarely provide impact estimates, such as the expected amount and distribution of physical damage, human consequences, disruption of services or financial loss. Complementing early warning systems with impact forecasts has a two‐fold advantage: it would provide decision makers with richer information to take informed decisions about emergency measures, and focus the attention of different disciplines on a common target. This would allow capitalizing on synergies between different disciplines and boosting the development of multi‐hazard early warning systems. This review discusses the state‐of‐the‐art in impact forecasting for a wide range of natural hazards. We outline the added value of impact‐based warnings compared to hazard forecasting for the emergency phase, indicate challenges and pitfalls, and synthesize the review results across hazard types most relevant for Europe. Plain language summary Forecasting and early warning systems are important investments to protect lives, properties and livelihood. While such systems are frequently used to predict the magnitude, location and timing of potentially damaging events, they rarely provide impact estimates, such as the expected physical damage, human consequences, disruption of services or financial loss. Extending hazard forecast systems to include impact estimates promises many benefits for the emergency phase, for instance, for organising evacuations. We review and compare the state‐of‐the‐art of impact forcasting across a wide range of natural hazards, and outline opportunities and key challenges for research and development of impact forecasting.

Description: A one‐dimensional reaction‐transport model is used to investigate the dynamics of methane gas in coastal sediments in response to intra‐annual variations in temperature and pressure. The model is applied to data from two shallow water sites in Eckernförde Bay (Germany) characterized by low and high rates of upward fluid advection. At both sites, organic matter is buried below the sulfate‐reducing zone to the methanogenic zone at sufficiently high rates to allow supersaturation of the pore water with dissolved methane and to form a free methane gas phase. The methane solubility concentration varies by similar magnitudes at both study sites in response to bottom water temperature changes and leads to pronounced peaks in the gas volume fraction in autumn when the methanic zone temperature is at a maximum. Yearly hydrostatic pressure variations have comparatively negligible effects on methane solubility. Field data suggest that no free gas escapes to the water column at any time of the year. Although the existence of gas migration cannot be substantiated by direct observation, a speculative mechanism for slow moving gas is proposed here. The model results reveal that free gas migrating upward into the undersaturated pore water will completely dissolve and subsequently be consumed above the free gas depth (FGD) by anaerobic oxidation of methane (AOM). This microbially mediated process maintains methane undersaturation above the FGD. Although the complexities introduced by seasonal changes in temperature lead to different seasonal trends for the depth‐integrated AOM rates and the FGD, both sites adhere to previously developed prognostic indicators for methane fluxes based on the FGD.

Description: Black carbon (BC) aerosols influence the Earth's atmosphere and climate, but their microphysical properties, spatiotemporal distribution, and long-range transport are not well constrained. This study presents airborne observations of the transatlantic transport of BC-rich African biomass burning (BB) smoke into the Amazon Basin using a Single Particle Soot Photometer (SP2) as well as several complementary techniques. We base our results on observations of aerosols and trace gases off the Brazilian coast onboard the HALO (High Altitude and LOng range) research aircraft during the ACRIDICON-CHUVA campaign in September 2014. During flight AC19 over land and ocean at the northeastern coastline of the Amazon Basin, we observed a BC-rich layer at ∼3.5 km altitude with a vertical extension of ∼0.3 km. Backward trajectories suggest that fires in African grasslands, savannas, and shrublands were the main source of this pollution layer and that the observed BB smoke had undergone more than 10 d of atmospheric transport and aging over the South Atlantic before reaching the Amazon Basin. The aged smoke is characterized by a dominant accumulation mode, centered at about 130 nm, with a particle concentration of Nacc=850±330 cm−3. The rBC particles account for ∼15 % of the submicrometer aerosol mass and ∼40 % of the total aerosol number concentration. This corresponds to a mass concentration range from 0.5 to 2 µg m−3 (1st to 99th percentiles) and a number concentration range from 90 to 530 cm−3. Along with rBC, high cCO (150±30 ppb) and cO3 (56±9 ppb) mixing ratios support the biomass burning origin and pronounced photochemical aging of this layer. Upon reaching the Amazon Basin, it started to broaden and to subside, due to convective mixing and entrainment of the BB aerosol into the boundary layer. Satellite observations show that the transatlantic transport of pollution layers is a frequently occurring process, seasonally peaking in August/September. By analyzing the aircraft observations together with the long-term data from the Amazon Tall Tower Observatory (ATTO), we found that the transatlantic transport of African BB smoke layers has a strong impact on the northern and central Amazonian aerosol population during the BB-influenced season (July to December). In fact, the early BB season (July to September) in this part of the Amazon appears to be dominated by African smoke, whereas the later BB season (October to December) appears to be dominated by South American fires. This dichotomy is reflected in pronounced changes in aerosol optical properties such as the single scattering albedo (increasing from 0.85 in August to 0.90 in November) and the BC-to-CO enhancement ratio (decreasing from 11 to 6 ng m−3 ppb−1). Our results suggest that, despite the high fraction of BC particles, the African BB aerosol acts as efficient cloud condensation nuclei (CCN), with potentially important implications for aerosol–cloud interactions and the hydrological cycle in the Amazon.

Description: Black carbon (BC) aerosols are influencing the Earth’s atmosphere and climate, but their microphysical properties, spatiotemporal distribution and long-range transport are not well constrained. This study analyzes the transatlantic transport of BC-rich African biomass burning (BB) pollution into the Amazon Basin, based on airborne observations of aerosol particles and trace gases in and off the Brazilian coast during the ACRIDICON-CHUVA campaign in September 2014, combining in-situ measurements on the research aircraft HALO with satellite remote-sensing and numerical model results. During flight AC19 over land and ocean at the Brazilian coastline in the northeast of the Amazon Basin, we observed a BC-rich atmospheric layer at ~ 3.5 km altitude with a vertical extension of ~ 0.3 km. Backward trajectory analyses suggest that fires in African grasslands, savannas, and shrublands were the main source of this pollution layer, and that the observed BB smoke had undergone more than 10 days of atmospheric transport and aging. The BC mass concentrations in the layer ranged from 0.5 to 2 μg m−3, and the BC particle number fraction of ~ 40 % was about 8 times higher than observed in a fresh Amazonian BB plume, representing the highest value ever observed in the region. Upon entering the Amazon Basin, the layer started to broaden and to subside, due to convective mixing and entrainment of the BB aerosol into the boundary layer. Satellite observations show that the transatlantic transport of pollution layers is a frequently occurring process, seasonally peaking in August/September. By analyzing the aircraft observations within the broader context of the long-term data from the Amazon Tall Tower Observatory (ATTO), we found that the transatlantic transport of African BB smoke layers has a strong impact on the north-central Amazonian aerosol population during the BB-influenced season (July to November). Specifically, the early BB season in this part of the Amazon appears to be dominated by African smoke, whereas the later BB season appears to be dominated by South American fires. This dichotomy is reflected in pronounced changes of aerosol optical properties such as the single scattering albedo (increasing from 0.85 in August to 0.90 in November) and the BC-to-CO enhancement ratio (decreasing from 7.4 to 4.4 ng m−3 ppb−1). Our results suggest that, despite the high amount of BC particles, the African BB aerosol act as efficient cloud condensation nuclei (CCN) with potentially important implications for aerosol-cloud interactions and the hydrological cycle in the Amazon Basin.

Description: Introduction to the SPARC Reanalysis Intercomparison Project (S-RIP) and overview of the reanalysis systems Masatomo Fujiwara, Jonathon S. Wright, Gloria L. Manney, Lesley J. Gray, James Anstey, Thomas Birner, Sean Davis, Edwin P. Gerber, V. Lynn Harvey, Michaela I. Hegglin, Cameron R. Homeyer, John A. Knox, Kirstin Krüger, Alyn Lambert, Craig S. Long, Patrick Martineau, Beatriz M. Monge-Sanz, Michelle L. Santee, Susann Tegtmeier, Simon Chabrillat, David G. H. Tan, David R. Jackson, Saroja Polavarapu, Gilbert P. Compo, Rossana Dragani, Wesley Ebisuzaki, Yayoi Harada, Chiaki Kobayashi, Will McCarty, Kazutoshi Onogi, Steven Pawson, Adrian Simmons, Krzysztof Wargan, Jeffrey S. Whitaker, and Cheng-Zhi Zou Atmos. Chem. Phys. Discuss., doi:10.5194/acp-2016-652,2016 Manuscript under review for ACP (discussion: open, 0 comments) We introduce the SPARC Reanalysis Intercomparison Project (S-RIP), review key concepts and elements of atmospheric reanalysis systems, and summarize the technical details of and differences among eleven of these systems. Our primary objective is to collect these items into a single reference that supports and streamlines scientific studies and intercomparisons of reanalysis products. We also address several common misunderstandings and points of confusion regarding reanalysis data sets.

Description: Introduction to the SPARC Reanalysis Intercomparison Project (S-RIP) and overview of the reanalysis systems Masatomo Fujiwara, Jonathon S. Wright, Gloria L. Manney, Lesley J. Gray, James Anstey, Thomas Birner, Sean Davis, Edwin P. Gerber, V. Lynn Harvey, Michaela I. Hegglin, Cameron R. Homeyer, John A. Knox, Kirstin Krüger, Alyn Lambert, Craig S. Long, Patrick Martineau, Beatriz M. Monge-Sanz, Michelle L. Santee, Susann Tegtmeier, Simon Chabrillat, David G. H. Tan, David R. Jackson, Saroja Polavarapu, Gilbert P. Compo, Rossana Dragani, Wesley Ebisuzaki, Yayoi Harada, Chiaki Kobayashi, Will McCarty, Kazutoshi Onogi, Steven Pawson, Adrian Simmons, Krzysztof Wargan, Jeffrey S. Whitaker, and Cheng-Zhi Zou Atmos. Chem. Phys. Discuss., doi:10.5194/acp-2016-652,2016 Manuscript under review for ACP (discussion: open, 0 comments) We introduce the SPARC Reanalysis Intercomparison Project (S-RIP), review key concepts and elements of atmospheric reanalysis systems, and summarize the technical details of and differences among eleven of these systems. Our primary objective is to collect these items into a single reference that supports and streamlines scientific studies and intercomparisons of reanalysis products. We also address several common misunderstandings and points of confusion regarding reanalysis data sets.

Description: The climate research community uses atmospheric reanalysis data sets to understand a wide range of processes and variability in the atmosphere, yet different reanalyses may give very different results for the same diagnostics. The Stratosphere–troposphere Processes And their Role in Climate (SPARC) Reanalysis Intercomparison Project (S-RIP) is a coordinated activity to compare reanalysis data sets using a variety of key diagnostics. The objectives of this project are to identify differences among reanalyses and understand their underlying causes, to provide guidance on appropriate usage of various reanalysis products in scientific studies, particularly those of relevance to SPARC, and to contribute to future improvements in the reanalysis products by establishing collaborative links between reanalysis centres and data users. The project focuses predominantly on differences among reanalyses, although studies that include operational analyses and studies comparing reanalyses with observations are also included when appropriate. The emphasis is on diagnostics of the upper troposphere, stratosphere, and lower mesosphere. This overview paper for the S-RIP special issue summarizes the motivation and goals of the S-RIP activity, and reviews key technical aspects of the reanalysis data sets that are the focus of the S-RIP report.

Description: Introduction to the SPARC Reanalysis Intercomparison Project (S-RIP) and overview of the reanalysis systems Masatomo Fujiwara, Jonathon S. Wright, Gloria L. Manney, Lesley J. Gray, James Anstey, Thomas Birner, Sean Davis, Edwin P. Gerber, V. Lynn Harvey, Michaela I. Hegglin, Cameron R. Homeyer, John A. Knox, Kirstin Krüger, Alyn Lambert, Craig S. Long, Patrick Martineau, Andrea Molod, Beatriz M. Monge-Sanz, Michelle L. Santee, Susann Tegtmeier, Simon Chabrillat, David G. H. Tan, David R. Jackson, Saroja Polavarapu, Gilbert P. Compo, Rossana Dragani, Wesley Ebisuzaki, Yayoi Harada, Chiaki Kobayashi, Will McCarty, Kazutoshi Onogi, Steven Pawson, Adrian Simmons, Krzysztof Wargan, Jeffrey S. Whitaker, and Cheng-Zhi Zou Atmos. Chem. Phys., 17, 1417-1452, doi:10.5194/acp-17-1417-2017, 2017 We introduce the SPARC Reanalysis Intercomparison Project (S-RIP), review key concepts and elements of atmospheric reanalysis systems, and summarize the technical details of and differences among 11 of these systems. This work supports scientific studies and intercomparisons of reanalysis products by collecting these background materials and technical details into a single reference. We also address several common misunderstandings and points of confusion regarding reanalyses.

Description: Introduction to the SPARC Reanalysis Intercomparison Project (S-RIP) and overview of the reanalysis systems Masatomo Fujiwara, Jonathon S. Wright, Gloria L. Manney, Lesley J. Gray, James Anstey, Thomas Birner, Sean Davis, Edwin P. Gerber, V. Lynn Harvey, Michaela I. Hegglin, Cameron R. Homeyer, John A. Knox, Kirstin Krüger, Alyn Lambert, Craig S. Long, Patrick Martineau, Andrea Molod, Beatriz M. Monge-Sanz, Michelle L. Santee, Susann Tegtmeier, Simon Chabrillat, David G. H. Tan, David R. Jackson, Saroja Polavarapu, Gilbert P. Compo, Rossana Dragani, Wesley Ebisuzaki, Yayoi Harada, Chiaki Kobayashi, Will McCarty, Kazutoshi Onogi, Steven Pawson, Adrian Simmons, Krzysztof Wargan, Jeffrey S. Whitaker, and Cheng-Zhi Zou Atmos. Chem. Phys., 17, 1417-1452, doi:10.5194/acp-17-1417-2017, 2017 We introduce the SPARC Reanalysis Intercomparison Project (S-RIP), review key concepts and elements of atmospheric reanalysis systems, and summarize the technical details of and differences among 11 of these systems. This work supports scientific studies and intercomparisons of reanalysis products by collecting these background materials and technical details into a single reference. We also address several common misunderstandings and points of confusion regarding reanalyses.

Description: The climate research community uses atmospheric reanalysis data sets to understand a wide range of processes and variability in the atmosphere, yet different reanalyses may give very different results for the same diagnostics. The Stratosphere–troposphere Processes And their Role in Climate (SPARC) Reanalysis Intercomparison Project (S-RIP) is a coordinated activity to compare reanalysis data sets using a variety of key diagnostics. The objectives of this project are to identify differences among reanalyses and understand their underlying causes, to provide guidance on appropriate usage of various reanalysis products in scientific studies, particularly those of relevance to SPARC, and to contribute to future improvements in the reanalysis products by establishing collaborative links between reanalysis centres and data users. The project focuses predominantly on differences among reanalyses, although studies that include operational analyses and studies comparing reanalyses with observations are also included when appropriate. The emphasis is on diagnostics of the upper troposphere, stratosphere, and lower mesosphere. This paper summarizes the motivation and goals of the S-RIP activity and extensively reviews key technical aspects of the reanalysis data sets that are the focus of this activity. The special issue The SPARC Reanalysis Intercomparison Project (S-RIP) in this journal serves to collect research with relevance to the S-RIP in preparation for the publication of the planned two (interim and full) S-RIP reports.

Description: Quantifying the precipitation within clouds is a crucial challenge to improve our current understanding of the Earth's hydrological cycle. We have investigated the relationship between the effective radius of droplets and ice particles (re) and precipitation water content (PWC) measured by cloud probes near the top of growing convective cumuli. The data for this study were collected during the ACRIDICON–CHUVA campaign on the HALO research aircraft in clean and polluted conditions over the Amazon Basin and over the western tropical Atlantic in September 2014. Our results indicate a threshold of re∼13 µm for warm rain initiation in convective clouds, which is in agreement with previous studies. In clouds over the Atlantic Ocean, warm rain starts at smaller re, likely linked to the enhancement of coalescence of drops formed on giant cloud condensation nuclei. In cloud passes where precipitation starts as ice hydrometeors, the threshold of re is also shifted to values smaller than 13 µm when coalescence processes are suppressed and precipitating particles are formed by accretion. We found a statistically significant linear relationship between PWC and re for measurements at cloud tops, with a correlation coefficient of ∼0.94. The tight relationship between re and PWC was established only when particles with sizes large enough to precipitate (drizzle and raindrops) are included in calculating re. Our results emphasize for the first time that re is a key parameter to determine both initiation and amount of precipitation at the top of convective clouds.

Description: Size-resolved measurements of atmospheric aerosol and cloud condensation nuclei (CCN) concentrations and hygroscopicity were conducted over a full seasonal cycle at the remote Amazon Tall Tower Observatory (ATTO, March 2014–February 2015). In a preceding companion paper, we presented annually and seasonally averaged data and parametrizations (Part 1; Pöhlker et al., 2016a). In the present study (Part 2), we analyze key features and implications of aerosol and CCN properties for the following characteristic atmospheric conditions: Empirically pristine rain forest (PR) conditions, where no influence of pollution was detectable, as observed during parts of the wet season from March to May. The PR episodes are characterized by a bimodal aerosol size distribution (strong Aitken mode with DAit ≈ 70 nm and NAit ≈ 160 cm−3, weak accumulation mode with Dacc ≈ 160 nm and Nacc≈ 90 cm−3), a chemical composition dominated by organic compounds, and relatively low particle hygroscopicity (κAit≈ 0.12, κacc ≈ 0.18). Long-range-transport (LRT) events, which frequently bring Saharan dust, African biomass smoke, and sea spray aerosols into the Amazon Basin, mostly during February to April. The LRT episodes are characterized by a dominant accumulation mode (DAit ≈ 80 nm, NAit ≈ 120 cm−3 vs. Dacc ≈ 180 nm, Nacc ≈ 310 cm−3), an increased abundance of dust and salt, and relatively high hygroscopicity (κAit≈ 0.18, κacc ≈ 0.35). The coarse mode is also significantly enhanced during these events. Biomass burning (BB) conditions characteristic for the Amazonian dry season from August to November. The BB episodes show a very strong accumulation mode (DAit ≈ 70 nm, NAit ≈ 140 cm−3 vs. Dacc ≈ 170 nm, Nacc ≈ 3400 cm−3), very high organic mass fractions (∼ 90 %), and correspondingly low hygroscopicity (κAit≈ 0.14, κacc ≈ 0.17). Mixed-pollution (MPOL) conditions with a superposition of African and Amazonian aerosol emissions during the dry season. During the MPOL episode presented here as a case study, we observed African aerosols with a broad monomodal distribution (D ≈ 130 nm, NCN,10 ≈ 1300 cm−3), with high sulfate mass fractions (∼ 20 %) from volcanic sources and correspondingly high hygroscopicity (κ100nm≈ 0.22), which were periodically mixed with fresh smoke from nearby fires (D ≈ 110 nm, NCN,10 ≈ 2800 cm−3) with an organic-dominated composition and sharply decreased hygroscopicity (κ150nm≈ 0.20). Insights into the aerosol mixing state are provided by particle hygroscopicity (κ) distribution plots, which indicate largely internal mixing for the PR aerosols (narrow κ distribution) and more external mixing for the BB, LRT, and MPOL aerosols (broad κ distributions). The CCN spectra (CCN concentration plotted against water vapor supersaturation) obtained for the different case studies indicate distinctly different regimes of cloud formation and microphysics depending on aerosol properties and meteorological conditions. The measurement results suggest that CCN activation and droplet formation in convective clouds are mostly aerosol-limited under PR and LRT conditions and updraft-limited under BB and MPOL conditions. Normalized CCN efficiency spectra (CCN divided by aerosol number concentration plotted against water vapor supersaturation) and corresponding parameterizations (Gaussian error function fits) provide a basis for further analysis and model studies of aerosol–cloud interactions in the Amazon.

Description: Along ultraslow spreading ridges melt is distributed unequally, but melt focusing guides melt away from amagmatic segments toward volcanic centers. An interplay of tectonism and magmatism is thought to control melt ascent, but the detailed process of melt extraction is not yet understood. We present a detailed image of the seismic velocity structure of the Logachev volcanic center and adjacent region along the Knipovich Ridge. With travel times of P- and S-waves of 3,959 earthquakes we performed a local earthquake tomography. We simultaneously inverted for source locations, velocity structure and the Vp/Vs-ratio. An extensive low velocity anomaly coincident with high Vp/Vs-ratios 〉1.9 lies underneath the volcanic center at depths of 10 km below sea level in an aseismic area. More shallow, tightly clustered earthquake swarms connect the anomaly to a shallow anomaly with high Vp/Vs-ratio beneath the basaltic seafloor. We consider the deep low-velocity anomaly to represent an area of partial melt from which melts ascent vertically to the surface and northwards into the adjacent segment. By comparing tomographic studies of the Logachev and Southwest Indian Ridge Segment-8 volcano we conclude that volcanic centers of ultraslow spreading ridges host spatially confined, circular partial melt areas below 10 km depth, in contrast to the shallow extended melt lenses along fast spreading ridges. Lateral feeding over distances of 35 km is possible at orthogonal spreading segments, but limited at the obliquely spreading Knipovich Ridge. Key Points - Active volcanic centers at ultraslow spreading ridges host deeper and more confined partial melt areas than faster spreading ridges - Earthquake swarms delineate melt ascent paths from the partial melt area to the surface - Lateral feeding at shallow depths into subordinate segments is prevented by ridge obliquity

Description: The Atlantic Tradewind Ocean-Atmosphere Mesoscale Interaction Campaign (ATOMIC) took place from 7 January to 11 July 2020 in the tropical North Atlantic between the eastern edge of Barbados and 51∘ W, the longitude of the Northwest Tropical Atlantic Station (NTAS) mooring. Measurements were made to gather information on shallow atmospheric convection, the effects of aerosols and clouds on the ocean surface energy budget, and mesoscale oceanic processes. Multiple platforms were deployed during ATOMIC including the NOAA RV Ronald H. Brown (RHB) (7 January to 13 February) and WP-3D Orion (P-3) aircraft (17 January to 10 February), the University of Colorado's Robust Autonomous Aerial Vehicle-Endurant Nimble (RAAVEN) uncrewed aerial system (UAS) (24 January to 15 February), NOAA- and NASA-sponsored Saildrones (12 January to 11 July), and Surface Velocity Program Salinity (SVPS) surface ocean drifters (23 January to 29 April). The RV Ronald H. Brown conducted in situ and remote sensing measurements of oceanic and atmospheric properties with an emphasis on mesoscale oceanic–atmospheric coupling and aerosol–cloud interactions. In addition, the ship served as a launching pad for Wave Gliders, Surface Wave Instrument Floats with Tracking (SWIFTs), and radiosondes. Details of measurements made from the RV Ronald H. Brown, ship-deployed assets, and other platforms closely coordinated with the ship during ATOMIC are provided here. These platforms include Saildrone 1064 and the RAAVEN UAS as well as the Barbados Cloud Observatory (BCO) and Barbados Atmospheric Chemistry Observatory (BACO). Inter-platform comparisons are presented to assess consistency in the data sets. Data sets from the RV Ronald H. Brown and deployed assets have been quality controlled and are publicly available at NOAA's National Centers for Environmental Information (NCEI) data archive (https://www.ncei.noaa.gov/archive/accession/ATOMIC-2020, last access: 2 April 2021). Point-of-contact information and links to individual data sets with digital object identifiers (DOIs) are provided herein.

Description: Spreading centers in the proximity of back‐rolling subduction zones constitute an ideal natural laboratory to investigate the interaction of magmatism and tectonism during the early evolution of back‐arc basins. Using 32 days of ocean bottom seismometer data, we located 697 microeathquakes at the southern Fonualei Rift and Spreading Center (S‐FRSC). The majority of epicenters concentrate along the central region of the axial valley, marking the active ridge axis. Only odd events were associated with the prominent faults bounding the axial valley. About 450 events are spatially clustered around 17°42’S and their waveforms show a pronounced similarity. Most of these events are associated with a 138 hours lasting earthquake swarm. The tectonic structure of the ridge axis in the S‐FRSC resembles a series of left‐stepping en echelon segments, expressed at the seafloor by numerous volcanic ridges. The recorded earthquake swarm is located at the stepover of two en echelon segments suggesting that the earthquake swarm is mainly tectonically driven. The events directly beneath our seismic network indicate a maximum depth of brittle faulting down to about 14 km below the seafloor. This is within the maximum depth range of brittle faulting at ultraslow mid‐ocean ridges. Since the thickness of the brittle lithosphere is mainly controlled by temperature, our results suggest a sub‐axial thermal structure similar to that of ultraslow mid‐ocean ridges of similar opening rates.

Description: Modelling the chemistry and transport of bromoform within a sea breeze driven convective system during the SHIVA Campaign Atmospheric Chemistry and Physics Discussions, 13, 20611-20676, 2013 Author(s): P. D. Hamer, V. Marécal, R. Hossaini, M. Pirre, N. Warwick, M. Chipperfield, A. A. Samah, N. Harris, A. Robinson, B. Quack, A. Engel, K. Krüger, E. Atlas, K. Subramaniam, D. Oram, E. Leedham, G. Mills, K. Pfeilsticker, S. Sala, T. Keber, H. Bönisch, L. K. Peng, M. S. M. Nadzir, P. T. Lim, A. Mujahid, A. Anton, H. Schlager, V. Catoire, G. Krysztofiak, S. Fühlbrügge, M. Dorf, and W. T. Sturges We carry out a case study of the transport and chemistry of bromoform and its product gases (PGs) in a sea breeze driven convective episode on 19 November 2011 along the North West coast of Borneo during the "Stratospheric ozone: Halogen Impacts in a Varying Atmosphere" (SHIVA) campaign. We use ground based, ship, aircraft and balloon sonde observations made during the campaign, and a 3-D regional online transport and chemistry model capable of resolving clouds and convection explicitly that includes detailed bromine chemistry. The model simulates the temperature, wind speed, wind direction fairly well for the most part, and adequately captures the convection location, timing, and intensity. The simulated transport of bromoform from the boundary layer up to 12 km compares well to aircraft observations to support our conclusions. The model makes several predictions regarding bromine transport from the boundary layer to the level of convective detrainment (11 to 12 km). First, the majority of bromine undergoes this transport as bromoform. Second, insoluble organic bromine carbonyl species are transported to between 11 and 12 km, but only form a small proportion of the transported bromine. Third, soluble bromine species, which include bromine organic peroxides, hydrobromic acid (HBr), and hypobromous acid (HOBr), are washed out efficiently within the core of the convective column. Fourth, insoluble inorganic bromine species (principally Br 2 ) are not washed out of the convective column, but are also not transported to the altitude of detrainment in large quantities. We expect that Br 2 will make a larger relative contribution to the total vertical transport of bromine atoms in scenarios with higher CHBr 3 mixing ratios in the boundary layer, which have been observed in other regions. Finally, given the highly detailed description of the chemistry, transport and washout of bromine compounds within our simulations, we make a series of recommendations about the physical and chemical processes that should be represented in 3-D chemical transport models (CTMs) and chemistry climate models (CCMs), which are the primary theoretical means of estimating the contribution made by CHBr 3 and other very short-lived substances (VSLS) to the stratospheric bromine budget.

Description: We carry out a case study of the transport and chemistry of bromoform and its product gases (PGs) in a sea breeze driven convective episode on 19 November 2011 along the North West coast of Borneo during the "Stratospheric ozone: Halogen Impacts in a Varying Atmosphere" (SHIVA) campaign. We use ground based, ship, aircraft and balloon sonde observations made during the campaign, and a 3-D regional online transport and chemistry model capable of resolving clouds and convection explicitly that includes detailed bromine chemistry. The model simulates the temperature, wind speed, wind direction fairly well for the most part, and adequately captures the convection location, timing, and intensity. The simulated transport of bromoform from the boundary layer up to 12 km compares well to aircraft observations to support our conclusions. The model makes several predictions regarding bromine transport from the boundary layer to the level of convective detrainment (11 to 12 km). First, the majority of bromine undergoes this transport as bromoform. Second, insoluble organic bromine carbonyl species are transported to between 11 and 12 km, but only form a small proportion of the transported bromine. Third, soluble bromine species, which include bromine organic peroxides, hydrobromic acid (HBr), and hypobromous acid (HOBr), are washed out efficiently within the core of the convective column. Fourth, insoluble inorganic bromine species (principally Br2) are not washed out of the convective column, but are also not transported to the altitude of detrainment in large quantities. We expect that Br2 will make a larger relative contribution to the total vertical transport of bromine atoms in scenarios with higher CHBr3 mixing ratios in the boundary layer, which have been observed in other regions. Finally, given the highly detailed description of the chemistry, transport and washout of bromine compounds within our simulations, we make a series of recommendations about the physical and chemical processes that should be represented in 3-D chemical transport models (CTMs) and chemistry climate models (CCMs), which are the primary theoretical means of estimating the contribution made by CHBr3 and other very short-lived substances (VSLS) to the stratospheric bromine budget.

Description: We evaluate modelled Antarctic ice sheet (AIS) near-surface climate, surface mass balance (SMB) and surface energy balance (SEB) from the updated polar version of the regional atmospheric climate model, RACMO2 (1979–2016). The updated model, referred to as RACMO2.3p2, incorporates upper-air relaxation, a revised topography, tuned parameters in the cloud scheme to generate more precipitation towards the AIS interior and modified snow properties reducing drifting snow sublimation and increasing surface snowmelt. Comparisons of RACMO2 model output with several independent observational data show that the existing biases in AIS temperature, radiative fluxes and SMB components are further reduced with respect to the previous model version. The model-integrated annual average SMB for the ice sheet including ice shelves (minus the Antarctic Peninsula, AP) now amounts to 2229 Gt y−1, with an interannual variability of 109 Gt y−1. The largest improvement is found in modelled surface snowmelt, which now compares well with satellite and weather station observations. For the high-resolution (∼ 5.5 km) AP simulation, results remain comparable to earlier studies. The updated model provides a new, high-resolution data set of the contemporary near-surface climate and SMB of the AIS; this model version will be used for future climate scenario projections in a forthcoming study.

Description: We evaluate modelled Antarctic ice sheet (AIS) near-surface climate, surface mass balance (SMB) and surface energy balance (SEB) from the updated polar version of the regional atmospheric climate model RACMO2 (1979–2016). The updated model, referred to as RACMO2.3p2, incorporates upper-air relaxation, a revised topography, tuned parameters in the cloud scheme to generate more precipitation towards the AIS interior, and modified snow properties reducing drifting snow sublimation and increasing surface snowmelt. Comparisons of RACMO2 model output with several independent observational data show that the existing biases in AIS temperature, radiative fluxes and SMB components are further reduced with respect to the previous model version. The model integrated annual average SMB for the ice sheet including ice shelves (minus the Antarctic Peninsula (AP)) now amounts to 2229 Gt y-1, with an interannual variability of 109 Gt y-1. The largest improvement is found in modelled surface snowmelt, that now compares well with satellite and weather station observations. For the high-resolution (~ 5.5 km) AP simulation, results remain comparable to earlier studies. The updated model provides a new, high-resolution dataset of the contemporary near-surface climate and SMB of the AIS; this model version will be used for future climate scenario projections in a forthcoming study.

Description: The stratospheric climate and variability from simulations of sixteen chemistryclimate models is evaluated. On average the polar night jet is well reproduced though its variability is less well reproduced with a large spread between models. Polar temperature biases are less than 5 K except in the Southern Hemisphere (SH) lower stratosphere in spring. The accumulated area of low temperatures responsible for polar stratospheric cloud formation is accurately reproduced for the Antarctic but underestimated for the Arctic. The shape and position of the polar vortex is well simulated, as is the tropical upwelling in the lower stratosphere. There is a wide model spread in the frequency of major sudden stratospheric warnings (SSWs), late biases in the breakup of the SH vortex, and a weak annual cycle in the zonal wind in the tropical upper stratosphere. Quantitatively, “metrics” indicate a wide spread in model performance for most diagnostics with systematic biases in many, and poorer performance in the SH than in the Northern Hemisphere (NH). Correlations were found in the SH between errors in the final warming, polar temperatures, the leading mode of variability, and jet strength, and in the NH between errors in polar temperatures, frequency of major SSWs, and jet strength. Models with a stronger QBO have stronger tropical upwelling and a colder NH vortex. Both the qualitative and quantitative analysis indicate a number of common and long‐standing model problems, particularly related to the simulation of the SH and stratospheric variability.

Description: Continuous high-resolution underway measurements of dimethyl sulfide (DMS) and isoprene in the ocean surface were conducted from Germany to South Africa in November 2008. DMS, total dimethylsulfoniopropionate (DMSPt), isoprene and 19'-hexanoyloxyfucoxanthin (19'-hex) correlated in nitrogen-depleted regions when they were clustered by nitrogen to phosphorous ratio (N:P). The 19'-hex-containing algae groups might be a common source of DMS, DMSPt, and isoprene in the low N: P regions. Additionally, DMS and isoprene correlated in nitrate-depleted regions when they were clustered against nitrate concentrations. Correlations between DMS and isoprene were also found within nitrate-depleted eddies encountered along the cruise track. Eddies with N: P of similar to 2.8 showed the highest positive correlations between DMS and isoprene. We conclude that the DMS/isoprene relationships in the eastern Atlantic Ocean were influenced by nutrient availability, with implications for using nutrients to predict the DMS and isoprene concentrations over a range of oceanographic areas depleted in nitrogen

Description: Stratospheric sudden warmings (SSWs) are extreme events in the polar stratosphere that are both caused by and have effects on the tropospheric flow. This means that SSWs are associated with changes in the angular momentum of the atmosphere, both before and after their onset. Because these angular momentum changes are transferred to the solid Earth, they can be observed in the rate of the Earth's rotation and the wobble of its rotational pole. By comparing observed Earth rotation variations to reanalysis data, we find that an anomaly in the orientation of the Earth's rotational pole, up to 4 times as large as the annual polar wobble, typically precedes SSWs by 20-40 days. The polar motion signal is due to pressure anomalies that are typically seen before SSW events and represents a new type of observable that may aid in the prediction of SSWs. A decline in the length of day is also seen, on average, near the time of the SSW wind reversal and is found to be due to anomalous easterly winds generated in the tropical troposphere around this time, though the structure and timing of this signal seems to vary widely from event to event.

Description: Since 2009, unprecedented comprehensive long-term gas hydrate observations have become available from Ocean Networks Canada's NEPTUNE cabled ocean observatory at the northern Cascadia margin. Several experiments demonstrate the scientific importance of permanent power and Internet connectivity to the ocean floor as they have advanced the field of gas hydrate related research. One example is the cabled crawler Wally at Barkley Canyon, enabling live in situ exploration of the hydrate mounds and its associated benthic communities through the crawler's mobility and permanent accessibility throughout the year. Another example is a bubble-imaging sonar at Clayoquot Slope, revealing the strong relationship between ebullition of natural gas and tidal pressure, without apparent correlation to earthquakes, storms, or temperature fluctuations, in year-long continuous recordings. Finally, regular observatory maintenance cruises allow additional science sampling including echo-sounder surveys to extend the observatory footprint. Long-term trends in the data are not yet apparent but can also become evident from continuous measurements, as ocean observatories such as NEPTUNE are built for a 25-year lifetime, and expansion of the observatory networks makes these findings comparable and testable. Plain Language Summary Natural gas near the ocean floor creates a rapidly changing environment where it is important to collect data continuously in order to determine the magnitude, speed, and potential mechanism of change. This long-standing challenge of year-round access to the deep ocean has been tackled by Ocean Networks Canada through cabling the northern Cascadia seafloor, providing power and Internet communication-ideal for power-hungry instruments, large data volumes, and real-time access. The presence of gas influences the shape of the seafloor, animal activity, and potential escape of methane, a potent greenhouse gas. A seafloor crawler Wally was operated around deep canyon mounds of gas hydrate (a solid gas-water composite) since 2009 and helped discover environmental changes influencing sea life. Further along the continental slope, an acoustic sonar monitored rising methane bubbles where the bubbling appears to be controlled neither by earthquakes, winter storms, nor subtle temperature changes but actually strongly by tidal pressure. Regular maintenance of the observatory by ship allows more data to be collected near the cabled seafloor sites, extending the observations to a larger area. Ocean observatories are built to last decades and therefore more data for more research can be collected, potentially detecting relatively slow processes as well.

Description: Oceanic emissions unlikely to account for the missing source of atmospheric carbonyl sulfide Sinikka T. Lennartz, Christa A. Marandino, Marc von Hobe, Pau Cortes, Birgit Quack, Rafel Simo, Dennis Booge, Andrea Pozzer, Tobias Steinhoff, Damian L. Arevalo-Martinez, Corinna Kloss, Astrid Bracher, Rüdiger Röttgers, Elliott Atlas, and Kirstin Krüger Atmos. Chem. Phys. Discuss., doi:10.5194/acp-2016-778,2016 Manuscript under review for ACP (discussion: open, 0 comments) We present new sea surface and marine boundary layer measurements of carbonyl sulfide, the most abundant sulfur gas in the atmosphere, and calculate an oceanic emission estimate. Our results imply that oceanic emissions are very unlikely to account for the missing source in the atmospheric budget that is currently discussed for OCS.

Description: Oceanic emissions unlikely to account for the missing source of atmospheric carbonyl sulfide Sinikka T. Lennartz, Christa A. Marandino, Marc von Hobe, Pau Cortes, Birgit Quack, Rafel Simo, Dennis Booge, Andrea Pozzer, Tobias Steinhoff, Damian L. Arevalo-Martinez, Corinna Kloss, Astrid Bracher, Rüdiger Röttgers, Elliott Atlas, and Kirstin Krüger Atmos. Chem. Phys. Discuss., doi:10.5194/acp-2016-778,2016 Manuscript under review for ACP (discussion: open, 0 comments) We present new sea surface and marine boundary layer measurements of carbonyl sulfide, the most abundant sulfur gas in the atmosphere, and calculate an oceanic emission estimate. Our results imply that oceanic emissions are very unlikely to account for the missing source in the atmospheric budget that is currently discussed for OCS.

Description: The climate active trace-gas carbonyl sulfide (OCS) is the most abundant sulfur gas in the atmosphere. A missing source in its atmospheric budget is currently suggested, resulting from an upward revision of the vegetation sink in top-down approaches. Oceanic emissions have been proposed to close the resulting gap in the atmospheric budget. We present a bottom-up approach including new observations of OCS in surface waters of the tropical Atlantic, Pacific and Indian oceans to show that direct OCS emissions are insufficient to account for the missing source. Extrapolation of our observations using a biogeochemical box model suggests oceanic net uptake instead of emission for the entire tropical ocean area and, further, a global ocean source strength well below that suggested by top-down estimates. This bottom-up estimate of oceanic emissions has implications for using OCS as a proxy for terrestrial CO2 uptake, which is currently hampered by the inadequate quantification of atmospheric OCS sources and sinks.

Description: In order to investigate the accuracy of simplification in modeling the radiative transfer in those solar spectral regions with major impacts on bio-organisms, i.e., the UVA (0.32–0.4 μm), the UVB (0.28–0.32 μm), and the photosynthetically active radiation (PAR, 0.4–0.7 μm), radiative transfer calculations with varying treatments of cloud geometries (plane-parallel homogeneous (PPHOM), independent column approximation (ICA), and three-dimensional (3-D) inhomogeneous) have been performed. The complete sets of atmospheric information for 133 cloud realizations are taken from the three-dimensional nonhydrostatic mesoscale atmospheric model (GESIMA). A Monte Carlo radiative transfer model (GRIMALDI) has been developed that simulates scattering and absorption for arbitrarily three-dimensional distributions of cloud hydrometeors, air molecules, and water vapor. Results are shown for domain-averaged direct and total transmission (and so, implicitly, diffuse transmission) at the ground surface. In the UVA the PPHOM assumption leads to an underestimation in direct (total) downward flux by as much as 43 (28) W m−2, which is about 49% (32%) of the incoming irradiation, whereas results based on the ICA are almost identical to the 3-D case, except for convective clouds where the error in the UVA for direct (total) downward flux reaches 5 (2) W m−2, or 6% (2%) of the incoming solar irradiation.

Description: We describe the main differences in simulations of stratospheric climate and variability by models within the fifth Coupled Model Intercomparison Project (CMIP5) that have a model top above the stratopause and relatively fine stratospheric vertical resolution (high-top), and those that have a model top below the stratopause (low-top). Although the simulation of mean stratospheric climate by the two model ensembles is similar, the low-top model ensemble has very weak stratospheric variability on daily and interannual time scales. The frequency of major sudden stratospheric warming events is strongly underestimated by the low-top models with less than half the frequency of events observed in the reanalysis data and high-top models. The lack of stratospheric variability in the low-top models affects their stratosphere-troposphere coupling, resulting in short-lived anomalies in the Northern Annular Mode, which do not produce long-lasting tropospheric impacts, as seen in observations. The lack of stratospheric variability, however, does not appear to have any impact on the ability of the low-top models to reproduce past stratospheric temperature trends. We find little improvement in the simulation of decadal variability for the high-top models compared to the low-top, which is likely related to the fact that neither ensemble produces a realistic dynamical response to volcanic eruptions

Description: A suite of oxygenated volatile organic compounds (OVOCs – acetaldehyde, acetone, propanal, butanal and butanone) were measured concurrently in the surface water and atmosphere of the South China Sea and Sulu Sea in November 2011. A strong correlation was observed between all OVOC concentrations in the surface seawater along the entire cruise track, except for acetaldehyde, suggesting similar sources and sinks in the surface ocean. Additionally, several phytoplankton groups, such as haptophytes or pelagophytes, were also correlated to all OVOCs indicating that phytoplankton may be an important source for marine OVOCs in the South China and Sulu Seas. Humic and protein like fluorescent dissolved organic matter (FDOM) components seemed to be additional precursors for butanone and acetaldehyde. The atmospheric OVOC mixing ratios were relative high compared with literature values, suggesting the coastal region of North Borneo as a local hot spot for atmospheric OVOCs. The flux of atmospheric OVOCs was largely into the ocean for all 5 gases, with a few important exceptions near the coast of Borneo. The calculated amount of OVOCs entrained into the ocean seemed to be an important source of OVOCs to the surface ocean. When the fluxes were out of the ocean, marine OVOCs were found to be enough to control the local measured OVOC distribution in the atmosphere. Based on our model calculations, at least 0.4 ppb of marine derived acetone and butanone can reach the upper troposphere, where they may have an important influence on hydrogen oxide radical formation over the western Pacific Ocean.

Description: Perturbations in stratospheric aerosol due to explosive volcanic eruptions are a primary contributor to natural climate variability. Observations of stratospheric aerosol are available for the past decades, and information from ice cores has been used to derive estimates of stratospheric sulfur injections and aerosol optical depth over the Holocene (approximately 10 000 BP to present) and into the last glacial period, extending back to 60 000 BP. Tephra records of past volcanism, compared to ice cores, are less complete but extend much further into the past. To support model studies of the potential impacts of explosive volcanism on climate variability across timescales, we present here an ensemble reconstruction of volcanic stratospheric sulfur injection (VSSI) over the last 140 000 years that is based primarily on terrestrial and marine tephra records. VSSI values are computed as a simple function of eruption magnitude based on VSSI estimates from ice cores and satellite observations for identified eruptions. To correct for the incompleteness of the tephra record, we include stochastically generated synthetic eruptions assuming a constant background eruption frequency from the ice core Holocene record. While the reconstruction often differs from ice core estimates for specific eruptions due to uncertainties in the data used and reconstruction method, it shows good agreement with an ice-core-based VSSI reconstruction in terms of millennial-scale cumulative VSSI variations over the Holocene. The PalVol reconstruction provides a new basis to test the contributions of forced vs. unforced natural variability to the spectrum of climate and the mechanisms leading to abrupt transitions in the palaeoclimate record with low- to high-complexity climate models. The PalVol volcanic forcing reconstruction is available at https://doi.org/10.26050/WDCC/PalVolv1 (Toohey and Schindlbeck-Belo, 2023).