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: 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: 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: 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: 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: 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: 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: 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: 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: 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: Within the Jeddah Transect Project, a multidisciplinary marine sampling program has been performed on RV Poseidon (P408 cruise) offshore Saudi-Arabia (Red Sea). The sampling program involved three projects (http://www.ifm-geomar.de/index.php?id=jeddahtransectdisc&L=1), covering aspects of marine petrology, biogeochemistry, oceanography and biology.

Description: The DRIVE (Diurnal and RegIonal Variability of Halogen Emissions) campaign to the eastern tropical North Atlantic Ocean and the upwelling off Mauritania (NW Africa) was funded by the BMBF as part of the German SOLAS project SOPRAN II (Surface Ocean Processes in the Anthropocene; www.sopran.pangaea.de): The second leg of the 399th cruise of R/V Poseidon (P399/2) took place from 31 May to 17 June 2010 (Las Palmas-Mindelo (Cape Verde Islands) – Mauritanian upwelling – Las Palmas). It was followed by the transit leg 3 (P399/3) which took place from 18 June to 24 June 2010 (Las Palmas – Vigo (Spain)) with only one stop at ESTOC. Ten scientists from IFM-GEOMAR (Kiel), IfAM (U Kiel), IfBM (U Hamburg) and IUP (U Heidelberg) representing various SOPRAN II subprojects took part in the cruise which was the sixth of a series of German SOLAS cruises to the tropical North Atlantic Ocean. The major objective of P399/2 was to investigate the regional and diurnal atmospheric and oceanic variations of halogenated compounds in the eastern tropical North Atlantic Ocean with a special focus on the Mauritanian upwelling. The main working packages of P399/2 and P399/3 included measurements of - Atmospheric BrO and IO - Atmospheric halocarbons - Other atmospheric trace gases such as ozone, methane etc. - Aerosol composition - Vertical structure of the atmosphere - Dissolved halocarbons, nitrous oxide and carbon dioxide - CTD, dissolved nutrients, O2, and chlorophyll - Microstructure of the upper water column Besides an extensive underway measurement program of dissolved (halocarbons, N2O, CO2) and atmospheric (BrO, halocarbons, other trace gases, aerosol) compounds, six 24h stations were performed and 23 regular CTD stations with depth profiles covering the entire water column were occupied.

Description: The evolution from the Western Mediterranean Sea is inherently governed by (i) plate convergence between Nubia (Africa) / Eurasia and (ii) subduction related slab-roll back. Both processes are responsible for the surface features / topography of the Gulf of Cadiz / Gibraltar Arc / Alboran Sea / Rif / Betic domain and deep-seated features related to the consumption of African lithosphere. The project is part of the ESF-EUROCORES programme TOPO-EUROPE and is aiming to study the interrelation between convergence and major tectonic fault zones in the Gulf of Cadiz and the Alboran Sea (Trans-Alboran- Shear-Zone – Alboran Ridge) and Miocene subduction / deep-seated seismicity at 40-150 km depth. Monitoring networks with ocean bottom seismometers (OBS) and hydrophones (OBH) were installed first in the Alboran Sea (August 2009 to January 2010) and later in the Gulf of Cadiz (January 2010 to July 2010), providing for the first time local earthquake data collected on ocean bottom stations. First results suggest that the collected data are of every good quality to assess seismotectonics in both domains and yielding travel time data for unique tomographic images of the Gibraltar arc area and Alboran domain, providing seismic constraints on the structure of crust and mantle.

Description: The cooperative research project between Chinese and German leading marine research institutions, the Guangzhou Marine Geological Survey (GMGS) and Leibniz-Institut für Meereswissenschaften Kiel (IFM-GEOMAR) addressed the geological methane budget and environmental effects of methane emissions from gas hydrates along the passive margin of the northern South China Sea. Two areas were surveyed of which the NE area (A) was sampled in great detail, whereas area B, after an initial survey, yielded less promising results. Swath map bathymetry, ocean floor observation by continuous video survey (OFOS) and water column methane distribution pattern provided the basis for locating several sites of ongoing methane venting. Outstanding among these was a methane-derived carbonate structure in water depths of 600-900m. Vast accumulations of vent carbonate debris, pavements and edifices standing above the seafloor characterize this structure. A 30-m high edifice, named Jiu Long Methane Reef, proved to be an active cold vent site with chemosynthetic fauna and bacterial mats. At deep sites ( apprx. 3000m) in and adjacent to the Formosa Canyon methane anomalies in the bottom water and clam colonies also indicate active methane venting. Pore water and gas chemistry on gravity cores indicated rather shallow depths of the sulfate-methane-interface (SMI) and documented chloride anomalies. High methane concentrations (exceeding 10.000 μM) in sediments, which when extrapolated, suggest that saturation might be reached at about 16-24 mbsf at which depths the shallowest gas hydrates might be encountered in the area. The project results contribute directly to several major science policy missions. (1) Documentation of vast amounts of methane emmited from the passive margin of the northern South China Sea is seen as evidence for long-term climate forcing by the greenhouse gas methane. (2) The functioning and significance of deep-sea biota as modulating the greenhouse gas budget is convincingly demonstrated by the vast amounts of methane carbon fixed as authigenic carbonates. (3) Further development of TV-guided deep-sea instrumentation, and above all the retrieval of undecompressed sediments, have again been deomonstrated as high a priority topic for the future of marine science. (4) The success of the project has demonstrated how international partnerships can efficiently been implemented.

Description: RV Sonne cruise 206 started on the 31st of May in Caldera (Costa Rica) and ended there on the 18th of June 2010. An international group of 23 scientists and 2 guests from Costa Rica set out to perform geophysical, biogeochemical, and sedimentological investigations at and around a number of submarine cold seeps that are ubiquitous along this convergent continental margin. The cruise was predominantly conducted as a pre-site survey for IODP (proposal 633Full-2; Costa Rica Mounds) in order to fill existing gaps in the seismic record at two of the proposed drill locations. A 2D seismic survey was conducted running over the large-scale seamount subduction slide “Jaco Scarp” yielding a highly improved image of the structural pattern within the upper 1000 m of the sedimentary sequence. In addition, high-resolution 3D seismic data, roughly covering the uppermost 300 m, could be obtained in the Mound 11/12 area, which will allow for a detailed analysis of the internal structure of these mud volcano-like features and help to understand the complex relation to the upward directed material flow. Moreover, a total number of 36 sediment cores (TV-guided multicorer, gravity corer) were successfully retrieved from active cold seeps and submarine slides and a large number of sub-samples were taken for subsequent geochemical and microbiological analyses. Overall, all major tasks of this cruise could successfully be fulfilled and the results will help to further our understanding of mechanisms controlling fluid flow in the deep subsurface of active continental margins.

Description: The research project SO208 PLUMEFLUX (Propagation of Galápagos Plume Material in the Equatorial East Pacific) is funded by the German Ministry of Education and Research (BMBF) and focusses on seamounts on the Cocos Plate, formed at the East Pacific Rise but presently located off the coast of NW Costa Rica and Nicaragua (Leg 1), and on the Cocos-Nazca-Spreading Center(CNS; Leg 2). The studies conducted on cruise SO208 included multi-beam mapping, sediment echo sounding, hard rock sampling, as well as sedimentological and biological sampling. The major geological targets of Leg 1 were (1) to evaluate if the seamounts off northern Costa Rica and Nicaragua were formed by the Galápagos hotspot and thus to constrain the extent of influence by the Galápagos plume on the upper asthenosphere and lithosphere and (2) to constrain better the material input into the Central American subduction zone. Leg 2 aimed to sample profiles of the seafloor perpendicular to the CNS using the mobile drill Rockdrill 2 of the British Geological Survey, in order to reconstruct plume-ridge interaction in the past to complement morphological, petrological and geochemical studies carried out on previous cruises along the ridge axis (e.g. SO158). The integration of the results with existing data should contribute towards a better understanding of transport processes of plume material in the upper mantle and of the geodynamic evolution of the central East Pacific. The sedimentological studies carried out on both Legs of SO208 focussed on radiolarian assemblages. SO208 startet in Caldera/Costa Rica on July 15th, 2010, and ended in Guayaquil/Ecuador on August 29th, 2010. During Leg 1 nineteen seamounts on the Cocos Plate have been mapped and sampled. Within only 12 days at sea, a total of 41 stations(28 dredges, 2 TV grabs, and 11 multicorers) were carried out. Of these deployments, 23 recovered magmatic rocks, 15 volcaniclastics, and 13 Mn-Fe oxides. The samples comprise mainly pillow and sheet lavas, often with fresh glassy margins, and a wide spectrum of volcaniclastic rocks. Notably, we found several indications for explosive volcanic activity at water depths 〉 3,000 m. Due to a series of unfortunate circumstances beyond our control, the planned Rockdrill 2 deployment on Leg 2 had to be cancelled. Instead we mapped and collected samples via dredging from 60 localities along five profiles perpendicular to CNS. A total of 83 stations (76 dredges, 3 TVgrabs, and 4 multicorers) were carried out. Of these deployments, 59 recovered magmatic rocks, 3 volcaniclastics, 51 volcanic glass, and 6 Mn-Fe oxides, making this a successful cruise despite the Rockdrill problem. The first and most detailed profile (with 23 sampled localities) extended from the ridge axis to the north at ~92°W. The morphology shows alternating regions of abyssal ridges and valleys (possibly reflecting less plume input into the ridge) and thicker elevated bands commonly containing seamounts, some of which are tectonically deformed (possibly reflecting axial ridge type morphology and thus greater plume input into the ridge). The second profile was carried out at the shallowest part of the ridge axis, closest to the hotspot, just to the east of the 91° Transform Fault. The third profile extended 30 km north of the ridge (at ~89°30´W), where a formerly on-axis seamount has been split in half. We want to evaluate how far in the past the unique enriched geochemical anomaly associated with the seamount persisted in the past. Thirteen sites were successfully sampled along a fourth profile at 89°10’W, extending 35 km north and 35 km south of the CNS into crust up to 500,000 yrs old. This site was selected, because a major depleted geochemical anomaly exists at that location. A final short profile was carried out to the north and south and east (on the ridge axis) of a lava plateau at 88°20’W that represents an enriched anomaly along the ridge axis. The morphology of the area studied on Leg 2 strongly suggests that the intensity of interaction of the plume with the ridge has varied considerably over the last several hundred thousand years along the entire part of the ridge that we studied. Geochemical data should allow us to constrain better variations in plume-ridge interaction through time. Biological material was obtained successfully as macrofauna and as sediment samples containing meiofaunal organisms with the help of a geological chain bag dredge, sediment traps, a multicorer and a TV-grab. Macrofaunal organisms were recovered at 93 out of 124 stations, 37 stations revealed sediment samples. During the cruise, a total of 8,598 meiofaunal organisms were centrifuged out of about 45 kg of sediment and sorted to animal group. Foraminifera and Nematoda dominated the meiofauna, followed by Copepoda and at a lower abundance by Tardigrada, Kinorhyncha and Loricifera. We also discovered a highly diverse benthic macrofauna, mainly represented by Porifera, Bryozoa, Annelida, Brachiopoda and even a few monoplacophoran molluscs.

Description: Cruise SO210 with RV SONNE to the active continental margin off Chile was conducted by shiptime exchange with RV METEOR. Funds for mobilizing the research team were provided by the German Science Foundation (DFG) in conjunction with the Collaborative Research Centre (SFB) 574 of the University of Kiel. In the first years, the SFB 574 investigated the pathways and fluxes of volatiles through the erosive subduction zone off Central America. For comparison, the studies were extended to the accretionary margin off Central Chile. Cruise SO210 is the last cruise conducted in the framework of SFB 574 and based on investigations of previous SFB-cruises on the RVs VIDAL GORMAZ and JAMES COOK. The first leg of cruise SO210 was dedicated to long gravity coring for volcanic ash layers from the erruptive Southern Volcanic Zone (SVZ) of the Andes that were either deposited as fallouts onto the incoming Nazca Plate or transported down the slope and across the Chile Trench. Eight gravity cores of 12 m length were retrieved seaward of the Chile Channel on the outer rise of the Nazca Plate. The second goal for coring was the description and dating of previously mapped submarine landslides as well as retrieval of slide-related material for geo-technical experiments. As the deployment frame for long coring had to be removed on the second leg we continued coring for mass-wasting and geochemistry with short cores. Ten gravity cores of 3 or 6 m barrel length were retrieved upslope of slides, the glide plane and redeposited material downslope of the slide evacuation area. This sampling activity was supported by detailed acoustic surveys with Parasound and multibeam to remap critical areas for mass wasting in search for events, e.g. triggered by the recent Mw 8.8 Maule Earthquake, such as flanks of submarine canyons or previously detected submarine slides and to fill data gaps in the existing bathymetric data. The major activity of the entire cruise was dedicated to the search and detailed sampling of manifestations of fluid discharge activity on the Chilean forearc. A total of 11 deployments with the video sled OFOS and 12 dives by the ROV KIEL 6000 were conducted for ground-truthing of information which indicated possible seep activity and has been obtained during previous cruises to the Chilean forearc. In five working areas we found manifestations of fluid discharge. In these areas the survey was followed by an intense sampling of bottom water, sediments, carbonates, mega and meiofauna and the deployment of instrumentation on the seafloor. The goal of these deployments was to measure in situ seabed methane emission rates and associated fluxes of sulfide and major electron acceptors such as oxygen at seep sites along the Chilean margin and to understand its controls. This was accompanied by CTD casts to trace oxygen and the fate of methane discharge in the water column. Sediment cores obtained by multicorer or ROV were used for the geochemical characterization of the pore water and microbiological studies which include turnover rate measurements, molecular studies, flow through experiments and sampling of active sediments. Authigenic carbonates obtained by TV-Grab or ROV were sampled for fauna, biomarker studies and investigations to reconstruct the growth structures, calcification processes and fluid-pathway systematic. The sampling of sediments and carbonates recovered a unique fauna with 79 different taxa, several of them appear to be species new to science.

Description: Cruise SO-214 of R/V SONNE headed by IFM-GEOMAR served two legs of project NEMESYS, funded through the German Ministry of Education and Research (BMBF). Major partners of the project are Leibniz Institute of Marine Science (IFM-GEOMAR) and the Federal Institute of Geosciences and Natural Resources (BGR) Germany, as well as the Institute of Geological and Nuclear Sciences (GNS) and the Royal Netherlands Institute for Sea Research (NIOZ). NEMESYS aims to extend understanding and modelling of cold vents along the Hikurangi Margin (HM) off the east coast of the North Island of New Zealand. Since the first findings in the late 80´s several cruises have been dedicated to map and investigate the active seepage of Methane in this area. Results of these cruises headed by New Zealand and international scientists provided the database for the first joint German – New Zealand expedition SO-191 in 2007. During this cruise with R/V SONNE the HM was investigated within three legs comprising all marine geo-scientific disciplines. The major findings in geophysical, geological, geo-chemical, and biological research were published in a special issue by Marine Geology (Vol. 272, 2010). Nevertheless a lot of questions remained or were raised by the upcoming results. Still lateral continuation of feeder channels and a possible relation between internal structure, activity and tectonic regime of a seep site were not understood. The geological, geo-chemical and biological analysis has been related to the overall description and study of the seep sites along the margin. Detailed studies across a seep site and high-resolution sampling to study the internal variation of Methane production and the influences to chemistry and habitat have not been complete with the required intensity. These exemplary listed investigations together with an additional list of questions to seepage led to the follow-up project SO-214 NEMESYS, which was funded through the German Ministry of Education and Research (BMBF). Aim of the project NEMESYS is to confirm derived models of seep structures and to extend the existing database and knowledge by high-resolution sampling in all disciplines. Based on the findings of the SO-191 New Vents project Opouawe Bank and Omakere Ridge were identified as the areas with the highest interest for our additional studies. Opouawe Bank provides a high density of active seep sites with various expressions of feeder channels in seismic images. Omakere did provide the only seep sites that were found without feeder channels underneath. In between the Porangahau Ridge was selected as third target due to the indications of either gas or hydrate formation without active gas expulsion. Cruise SO-214 with R/V SONNE was split into two legs. The seismic part started on 09th March 2011 in the port of Wellington. Two 3D seismic cubes were acquired above active seep sites at Omakere and Opouawe Bank. A third cube at Porangahau Ridge could not be completed due to technical problems with the equipment and rough weather conditions. Intensive Parasound Profiling and extended 2D seismic with high resolution (up to 1.2 m migration grid) were undertaken. Many more feeder channels were identified than previously known from the SO-191 data, although not all of them terminate in a seafloor expression. The second leg left the port of Wellington on 6th April 2011 dedicated to intensive geological, geo-chemical and biological investigations. The major work was completed at Opouawe Bank. Based on images of the seismic data compilation North and South Tower seeps and seep site Takahe were chosen for the intensive sampling program. CTD and gravity cores were taken in dense spacing to investigate the local interaction of seepage and surrounding seafloor and water column. The water column showed limited stratification but seemed to be influenced from stormy weather. Biologic investigations showed limited variations compared with the SO-191 expedition, mainly in the distribution of fauna. The variety of amphipods seems to be a unique feature of the NZ seeps. The second leg suffered from bad weather conditions, which anticipated work during 100 hrs. out of scheduled 330 hrs. All meta data of the cruise are available through the IFM-GEOMAR Data Management Portal (https://portal.ifm-geomar.de/web/guest/home)

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: 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.