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  • 1
    Publication Date: 2020-02-06
    Description: Reanalysis data sets are widely used to understand atmospheric processes and past variability, and are often used to stand in as "observations" for comparisons with climate model output. Because of the central role of water vapor (WV) and ozone (O3) in climate change, it is important to understand how accurately and consistently these species are represented in existing global reanalyses. In this paper, we present the results of WV and O3 intercomparisons that have been performed as part of the SPARC (Stratosphere–troposphere Processes and their Role in Climate) Reanalysis Intercomparison Project (S-RIP). The comparisons cover a range of timescales and evaluate both inter-reanalysis and observation-reanalysis differences. We also provide a systematic documentation of the treatment of WV and O3 in current reanalyses to aid future research and guide the interpretation of differences amongst reanalysis fields. The assimilation of total column ozone (TCO) observations in newer reanalyses results in realistic representations of TCO in reanalyses except when data coverage is lacking, such as during polar night. The vertical distribution of ozone is also relatively well represented in the stratosphere in reanalyses, particularly given the relatively weak constraints on ozone vertical structure provided by most assimilated observations and the simplistic representations of ozone photochemical processes in most of the reanalysis forecast models. However, significant biases in the vertical distribution of ozone are found in the upper troposphere and lower stratosphere in all reanalyses. In contrast to O3, reanalysis estimates of stratospheric WV are not directly constrained by assimilated data. Observations of atmospheric humidity are typically used only in the troposphere, below a specified vertical level at or near the tropopause. The fidelity of reanalysis stratospheric WV products is therefore mainly dependent on the reanalyses' representation of the physical drivers that influence stratospheric WV, such as temperatures in the tropical tropopause layer, methane oxidation, and the stratospheric overturning circulation. The lack of assimilated observations and known deficiencies in the representation of stratospheric transport in reanalyses result in much poorer agreement amongst observational and reanalysis estimates of stratospheric WV. Hence, stratospheric WV products from the current generation of reanalyses should generally not be used in scientific studies.
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  • 2
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    Copernicus Publications (EGU)
    In:  Atmospheric Chemistry and Physics, 17 (18). pp. 11313-11329.
    Publication Date: 2020-02-06
    Description: Very short-lived substances (VSLS) contribute as source gases significantly to the tropospheric and stratospheric bromine loading. At present, an estimated 25% of stratospheric bromine is of oceanic origin. In this study, we investigate how climate change may impact the ocean- atmosphere flux of brominated VSLS, their atmospheric transport, and chemical transformations and evaluate how these changes will affect stratospheric ozone over the 21st century. Under the assumption of fixed ocean water concentrations and RCP6.0 scenario, we find an increase of the ocean- atmosphere flux of brominated VSLS of about 8-10% by the end of the 21st century compared to present day. A decrease in the tropospheric mixing ratios of VSLS and an increase in the lower stratosphere are attributed to changes in atmospheric chemistry and transport. Our model simulations reveal that this increase is counteracted by a corresponding reduction of inorganic bromine. Therefore the total amount of bromine from VSLS in the stratosphere will not be changed by an increase in upwelling. Part of the increase of VSLS in the tropical lower stratosphere results from an increase in the corresponding tropopause height. As the depletion of stratospheric ozone due to bromine depends also on the availability of chlorine, we find the impact of bromine on stratospheric ozone at the end of the 21st century reduced compared to present day. Thus, these studies highlight the different factors influencing the role of brominated VSLS in a future climate
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  • 3
    Publication Date: 2020-02-06
    Description: Carbohydrates represent an important fraction of labile and semi-labile marine organic matter that is mainly comprised of exopolymeric substances derived from phytoplankton exudation and decay. This study investigates the composition of total combined carbohydrates (tCCHO; 〉1 kDa) and the community development of free-living (0.2–3 μm) and particle-associated (PA) (3–10 μm) bacterioplankton during a spring phytoplankton bloom in the southern North Sea. Furthermore, rates were determined for the extracellular enzymatic hydrolysis that catalyzes the initial step in bacterial organic matter remineralization. Concentrations of tCCHO greatly increased during bloom development, while the composition showed only minor changes over time. The combined concentration of glucose, galactose, fucose, rhamnose, galactosamine, glucosamine, and glucuronic acid in tCCHO was a significant factor shaping the community composition of the PA bacteria. The richness of PA bacteria greatly increased in the post-bloom phase. At the same time, the increase in extracellular β-glucosidase activity was sufficient to explain the observed decrease in tCCHO, indicating the efficient utilization of carbohydrates by the bacterioplankton community during the post-bloom phase. Our results suggest that carbohydrate concentration and composition are important factors in the multifactorial environmental control of bacterioplankton succession and the enzymatic hydrolysis of organic matter during phytoplankton blooms.
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  • 4
    Publication Date: 2021-07-08
    Description: Halogenated very short-lived substances (VSLSs) are naturally produced in the ocean and emitted to the atmosphere. When transported to the stratosphere, these compounds can have a significant influence on the ozone layer and climate. During a research cruise on RV Sonne in the subtropical and tropical west Indian Ocean in July and August 2014, we measured the VSLSs, methyl iodide (CH3I) and for the first time bromoform (CHBr3) and dibromomethane (CH2Br2), in surface seawater and the marine atmosphere to derive their emission strengths. Using the Lagrangian particle dispersion model FLEXPART with ERA-Interim meteorological fields, we calculated the direct contribution of observed VSLS emissions to the stratospheric halogen burden during the Asian summer monsoon. Furthermore, we compare the in situ calculations with the interannual variability of transport from a larger area of the west Indian Ocean surface to the stratosphere for July 2000–2015. We found that the west Indian Ocean is a strong source for CHBr3 (910 pmol m−2 h−1), very strong source for CH2Br2 (930 pmol m−2 h−1), and an average source for CH3I (460 pmol m−2 h−1). The atmospheric transport from the tropical west Indian Ocean surface to the stratosphere experiences two main pathways. On very short timescales, especially relevant for the shortest-lived compound CH3I (3.5 days lifetime), convection above the Indian Ocean lifts oceanic air masses and VSLSs towards the tropopause. On a longer timescale, the Asian summer monsoon circulation transports oceanic VSLSs towards India and the Bay of Bengal, where they are lifted with the monsoon convection and reach stratospheric levels in the southeastern part of the Asian monsoon anticyclone. This transport pathway is more important for the longer-lived brominated compounds (17 and 150 days lifetime for CHBr3 and CH2Br2). The entrainment of CHBr3 and CH3I from the west Indian Ocean to the stratosphere during the Asian summer monsoon is lower than from previous cruises in the tropical west Pacific Ocean during boreal autumn and early winter but higher than from the tropical Atlantic during boreal summer. In contrast, the projected CH2Br2 entrainment was very high because of the high emissions during the west Indian Ocean cruise. The 16-year July time series shows highest interannual variability for the shortest-lived CH3I and lowest for the longest-lived CH2Br2. During this time period, a small increase in VSLS entrainment from the west Indian Ocean through the Asian monsoon to the stratosphere is found. Overall, this study confirms that the subtropical and tropical west Indian Ocean is an important source region of halogenated VSLSs, especially CH2Br2, to the troposphere and stratosphere during the Asian summer monsoon.
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  • 5
    Publication Date: 2020-02-06
    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.
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  • 6
    Publication Date: 2020-10-26
    Description: Coastal seas may account for more than 75 % of global oceanic methane emissions. There, methane is mainly produced microbially in anoxic sediments from where it can escape to the overlying water column. Aerobic methane oxidation (MOx) in the water column acts as a biological filter reducing the amount of methane that eventually evades to the atmosphere. The efficiency of the MOx filter is potentially controlled by the availability of dissolved methane and oxygen, as well as temperature, salinity, and hydrographic dynamics, and all of these factors undergo strong temporal fluctuations in coastal ecosystems. In order to elucidate the key environmental controls, specifically the effect of oxygen availability, on MOx in a seasonally stratified and hypoxic coastal marine setting, we conducted a 2-year time-series study with measurements of MOx and physico-chemical water column parameters in a coastal inlet in the southwestern Baltic Sea (Eckernförde Bay). We found that MOx rates always increased toward the seafloor, but were not directly linked to methane concentrations. MOx exhibited a strong seasonal variability, with maximum rates (up to 11.6 nmol l−1 d−1) during summer stratification when oxygen concentrations were lowest and bottom-water temperatures were highest. Under these conditions, 70–95 % of the sediment-released methane was oxidized, whereas only 40–60 % were consumed during the mixed and oxygenated periods. Laboratory experiments with manipulated oxygen concentrations in the range of 0.2–220 µmol l−1 revealed a sub-micromolar oxygen-optimum for MOx at the study site. In contrast, the fraction of methane-carbon incorporation into the bacterial biomass (compared to the total amount of oxidised methane) was up to 38-fold higher at saturated oxygen concentrations, suggesting a different partitioning of catabolic and anabolic processes under oxygen-replete and oxygen-starved conditions, respectively. Our results underscore the importance of MOx in mitigating methane emission from coastal waters and indicate an organism-level adaptation of the water column methanotrophs to hypoxic conditions.
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  • 7
    Publication Date: 2017-09-09
    Description: Peter T. Witkowski, Casey C. Perley, Rebecca L. Brocato, Jay W. Hooper, Christian Jürgensen, Jörg-Dieter Schulzke, Detlev H. Krüger, Roland Bücker
    Electronic ISSN: 1664-302X
    Topics: Biology
    Published by Frontiers
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  • 8
    Publication Date: 2020-02-06
    Description: It is well established that variable wintertime planetary wave forcing in the stratosphere controls the variability of Arctic stratospheric ozone through changes in the strength of the polar vortex and the residual circulation. While previous studies focused on the variations in upward wave flux entering the lower stratosphere, here the impact of downward planetary wave reflection on ozone is investigated for the first time. Utilizing the MERRA2 reanalysis and a fully coupled chemistry–climate simulation with the Community Earth System Model (CESM1(WACCM)) of the National Center for Atmospheric Research (NCAR), we find two downward wave reflection effects on ozone: (1) the direct effect in which the residual circulation is weakened during winter, reducing the typical increase of ozone due to upward planetary wave events and (2) the indirect effect in which the modification of polar temperature during winter affects the amount of ozone destruction in spring. Winter seasons dominated by downward wave reflection events (i.e., reflective winters) are characterized by lower Arctic ozone concentration, while seasons dominated by increased upward wave events (i.e., absorptive winters) are characterized by relatively higher ozone concentration. This behavior is consistent with the cumulative effects of downward and upward planetary wave events on polar stratospheric ozone via the residual circulation and the polar temperature in winter. The results establish a new perspective on dynamical processes controlling stratospheric ozone variability in the Arctic by highlighting the key role of wave reflection.
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  • 9
    Publication Date: 2020-02-06
    Description: The microbial community response to petroleum seepage was investigated in a whole round sediment core (16 cm length) collected nearby natural hydrocarbon seepage structures in the Caspian Sea, using a newly developed Sediment-Oil-Flow-Through (SOFT) system. Distinct redox zones established and migrated vertically in the core during the 190 days-long simulated petroleum seepage. Methanogenic petroleum degradation was indicated by an increase in methane concentration from 8 μM in an untreated core compared to 2300 μM in the lower sulfate-free zone of the SOFT core at the end of the experiment, accompanied by a respective decrease in the δ13C signal of methane from -33.7 to -49.5‰. The involvement of methanogens in petroleum degradation was further confirmed by methane production in enrichment cultures from SOFT sediment after the addition of hexadecane, methylnapthalene, toluene, and ethylbenzene. Petroleum degradation coupled to sulfate reduction was indicated by the increase of integrated sulfate reduction rates from 2.8 SO42-m-2 day-1 in untreated cores to 5.7 mmol SO42-m-2 day-1 in the SOFT core at the end of the experiment, accompanied by a respective accumulation of sulfide from 30 to 447 μM. Volatile hydrocarbons (C2–C6 n-alkanes) passed through the methanogenic zone mostly unchanged and were depleted within the sulfate-reducing zone. The amount of heavier n-alkanes (C10–C38) decreased step-wise toward the top of the sediment core and a preferential degradation of shorter (〈C14) and longer chain n-alkanes (〉C30) was seen during the seepage. This study illustrates, to the best of our knowledge, for the first time the development of methanogenic petroleum degradation and the succession of benthic microbial processes during petroleum passage in a whole round sediment core.
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  • 10
    Publication Date: 2020-02-06
    Description: At the end of 2014, a Major Baltic Inflow (MBI) brought oxygenated, salty water into the Baltic proper and reached the long-term anoxic Eastern Gotland Basin (EGB) by March 2015. In July 2015, we measured benthic fluxes of phosphorus (P), nitrogen (N) and silicon (Si) nutrients and dissolved inorganic carbon (DIC) in situ using an autonomous benthic lander at deep sites (170-210 m) in the EGB, where the bottom water oxygen concentration was 30-45 μM. The same in situ methodology was used to measure benthic fluxes at the same sites in 2008-2010, but then under anoxic conditions. The high efflux of phosphate under anoxic conditions became lower upon oxygenation, and turned into an influx in about 50% of the flux measurements. The C:P and N:P ratios of the benthic solute flux changed from clearly below the Redfield ratio (on average about 70 and 3-4, respectively) under anoxia to approaching or being well above the Redfield ratio upon oxygenation. These observations demonstrate retention of P in newly oxygenated sediments. We found no significant effect of oxygenation on the benthic ammonium, silicate and DIC flux. We also measured benthic denitrification, anammox, and dissimilatory nitrate reduction to ammonium (DNRA) rates at the same sites using isotope-pairing techniques. The bottom water of the long-term anoxic EGB contained less than 0.5 μM nitrate in 2008-2010, but the oxygenation event created bottom water nitrate concentrations of about 10 μM in July 2015 and the benthic flux of nitrate was consistently directed into the sediment. Nitrate reduction to both dinitrogen gas (denitrification) and ammonium (DNRA) was initiated in the newly oxygenated sediments, while anammox activity was negligible. We estimated the influence of this oxygenation event on the magnitudes of the integrated benthic P flux (the internal P load) and the fixed N removal through benthic and pelagic denitrification by comparing with a hypothetical scenario without the MBI. Our calculations suggest that the oxygenation triggered by the MBI in July 2015, extrapolated to the basin-wide scale of the Baltic proper, decreased the internal P load by 23% and increased the total (benthic plus pelagic) denitrification by 18%.
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  • 11
    Publication Date: 2020-02-06
    Description: The climate research community uses atmospheric reanalysis data sets to understand a wide range of processes and variability in the atmosphere, yet different reanalyses may give very different results for the same diagnostics. The Stratosphere–troposphere Processes And their Role in Climate (SPARC) Reanalysis Intercomparison Project (S-RIP) is a coordinated activity to compare reanalysis data sets using a variety of key diagnostics. The objectives of this project are to identify differences among reanalyses and understand their underlying causes, to provide guidance on appropriate usage of various reanalysis products in scientific studies, particularly those of relevance to SPARC, and to contribute to future improvements in the reanalysis products by establishing collaborative links between reanalysis centres and data users. The project focuses predominantly on differences among reanalyses, although studies that include operational analyses and studies comparing reanalyses with observations are also included when appropriate. The emphasis is on diagnostics of the upper troposphere, stratosphere, and lower mesosphere. This paper summarizes the motivation and goals of the S-RIP activity and extensively reviews key technical aspects of the reanalysis data sets that are the focus of this activity. The special issue "The SPARC Reanalysis Intercomparison Project (S-RIP)" in this journal serves to collect research with relevance to the S-RIP in preparation for the publication of the planned two (interim and full) S-RIP reports.
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  • 12
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    Copernicus Publications (EGU)
    In:  Biogeosciences (BG), 14 (6). pp. 1349-1364.
    Publication Date: 2020-02-06
    Description: Ocean eddies can both trigger mixing (during their formation and decay) and effectively shield water encompassed from being exchanged with ambient water (throughout their lifetimes). These antagonistic effects of eddies complicate the interpretation of synoptic snapshots typically obtained by ship-based oceanographic measurement campaigns. Here we use a coupled physical–biogeochemical model to explore biogeochemical dynamics within anticyclonic eddies in the eastern tropical South Pacific Ocean. The goal is to understand the diverse biogeochemical patterns that have been observed at the subsurface layers of the anticyclonic eddies in this region. Our model results suggest that the diverse subsurface nutrient patterns within eddies are associated with the presence of water masses of different origins at different depths.
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  • 13
    Publication Date: 2020-02-06
    Description: Redox-sensitive mobilization of nutrients from sediments strongly affects the eutrophic state of the central Baltic Sea; a region associated with the spread of hypoxia and almost permanently anoxic and sulfidic conditions in the deeper basins. Ventilation of these basins depends on renewal by inflow of water enriched in oxygen (O2) from the North Sea, occurring roughly once per decade. Benthic fluxes and water column distributions of dissolved inorganic nitrogen species, phosphate (PO43-), dissolved inorganic carbon (DIC), sulfide (HS-), and total oxygen uptake (TOU) were measured along a depth gradient in the Eastern Gotland Basin (EGB). Campaigns were conducted during euxinic conditions of the deep basin in Aug./Sept. 2013 and after two inflow events in July/Aug. 2015 and March 2016 when O2 concentrations in deep waters reached 60 μM. The intrusion of O2-rich North Sea water into the EGB led to an approximate 33 and 10% reduction of the seabed PO43- and ammonium (NH4+) release from deep basin sediments. Post-inflow, the deep basin sediment was rapidly colonized by HS- oxidizing bacteria tentatively assigned to the family Beggiatoaceae, and HS- release was completely suppressed. The presence of a hypoxic transition zone (HTZ) between 80 and 120 m water depth was confirmed not only for euxinic deep-water conditions during 2013 but also for post-inflow conditions. Because deep-water renewal did not ventilate the HTZ, where PO43- and NH4+ fluxes were highest, high seabed nutrient release there was relatively unchanged. Extrapolation of the in situ nutrient fluxes indicated that, overall, the reduction in PO43- and NH4+ release in response to deep-water renewal can be considered as minor, reducing the internal nutrient load by 2 and 12% only, respectively. Infrequent inflow events thus have a limited capacity to sustainably reduce internal nutrient loading in the EGB and mitigate eutrophication.
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  • 14
    Publication Date: 2023-09-19
    Description: Water masses influenced by oxygen minimum zones (OMZ) feature low inorganic nitrogen (N) to phosphorus (P) ratios. The surplus of P over N is thought to favor non-Redfield primary production by bloom-forming phytoplankton species. Additionally, excess phosphate (P*) is thought to provide a niche for nitrogen fixing organisms. In order to assess the effect of low inorganic nutrient ratios on the stoichiometry and composition of primary producers, biogeochemical measurements were carried out in 2012 during a research cruise in the eastern tropical South Pacific (ETSP). Based on pigment analyses, a succession of different phytoplankton functional groups was observed along onshore—offshore transects with diatoms dominating the productive upwelling region, and prymnesiophytes, cryptophytes, and Synechococcus prevailing in the oligotrophic open ocean. Although inorganic nutrient supply ratios were below Redfield proportions throughout the sampling area, the stoichiometry of particulate organic nitrogen to phosphorus (PON:POP) generally exceeded ratios of 16:1. Despite PON:POP ≥ 16, high P*-values in the surface layer (0–50 m) above the shelf rapidly decreased as water masses were advected offshore. There are three mechanisms which can explain these observations: (1) non-Redfield primary production, where the excess phosphorus in the biomass is directly released as dissolved organic phosphorus (DOP), (2) non-Redfield primary production, which is masked by a particulate organic matter pool mainly consisting of P-depleted detrital biomass, and/or (3) Redfield primary production combined with dinitrogen (N2) fixation. Our observations suggest that the three processes occur simultaneously in the study area; quantifying the relative importance of each of these mechanisms needs further investigation. Therefore, it remains uncertain whether the ETSP is a net sink for bioavailable N or whether the N-deficit in this area is replenished locally.
    Type: Article , PeerReviewed , info:eu-repo/semantics/article
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  • 15
    Publication Date: 2020-02-06
    Description: Anaerobic microbial hydrocarbon degradation is a major biogeochemical process at marine seeps. Here we studied the response of the microbial community to petroleum seepage simulated for 190 days in a sediment core from the Caspian Sea using a sediment-oil-flow-through (SOFT) system. Untreated (without simulated petroleum seepage) and SOFT sediment microbial communities shared 43% bacterial genuslevel 16S rRNA-based operational taxonomic units (OTU0:945) but shared only 23% archaeal OTU0:945. The community differed significantly between sediment layers. The detection of fourfold higher deltaproteobacterial cell numbers in SOFT than in untreated sediment at depths characterized by highest sulfate reduction rates and strongest decrease of gaseous and mid-chain alkane concentrations indicated a specific response of hydrocarbon-degrading Deltaproteobacteria. Based on an increase in specific CARD-FISH cell numbers, we suggest the following groups of sulfate-reducing bacteria to be likely responsible for the observed decrease in aliphatic and aromatic hydrocarbon concentration in SOFT sediments: clade SCA1 for propane and butane degradation, clade LCA2 for mid- to long-chain alkane degradation, clade Cyhx for cycloalkanes, pentane and hexane degradation, and relatives of Desulfobacula for toluene degradation. Highest numbers of archaea of the genus Methanosarcina were found in the methanogenic zone of the SOFT core where we detected preferential degradation of long-chain hydrocarbons. Sequencing of masD, a marker gene for alkane degradation encoding (1-methylalkyl)succinate synthase, revealed a low diversity in SOFT sediment with two abundant species-level MasD OTU0:96.
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  • 16
    Publication Date: 2020-02-06
    Description: The sediment-water interface is an important site for material exchange in marine systems and harbor unique microbial habitats. The flux of nutrients, metals, and greenhouse gases at this interface may be severely dampened by the activity of microorganisms and abiotic redox processes, leading to the “benthic filter” concept. In this study, we investigate the spatial variability, mechanisms and quantitative importance of a microbially-dominated benthic filter for dissolved sulfide in the Eastern Gotland Basin (Baltic Sea) that is located along a dynamic redox gradient between 65 and 173 m water depth. In August-September 2013, high resolution (0.25 mm minimum) vertical microprofiles of redox-sensitive species were measured in surface sediments with solid-state gold-amalgam voltammetric microelectrodes. The highest sulfide consumption (2.73–3.38 mmol m−2 day−1) occurred within the top 5 mm in sediments beneath a pelagic hypoxic transition zone (HTZ, 80–120 m water depth) covered by conspicuous white bacterial mats of genus Beggiatoa. A distinct voltammetric signal for polysulfides, a transient sulfur oxidation intermediate, was consistently observed within the mats. In sediments under anoxic waters (〉140 m depth), signals for Fe(II) and aqueous FeS appeared below a subsurface maximum in dissolved sulfide, indicating a Fe(II) flux originating from older sediments presumably deposited during the freshwater Ancylus Lake that preceded the modern Baltic Sea. Our results point to a dynamic benthic sulfur cycling in Gotland Basin where benthic sulfide accumulation is moderated by microbial sulfide oxidation at the sediment surface and FeS precipitation in deeper sediment layers. Upscaling our fluxes to the Baltic Proper; we find that up to 70% of the sulfide flux (2281 kton yr−1) toward the sediment-seawater interface in the entire basin can be consumed at the microbial mats under the HTZ (80–120 m water depth) while only about 30% the sulfide flux effuses to the bottom waters (〉120 m depth). This newly described benthic filter for the Gotland Basin must play a major role in limiting the accumulation of sulfide in and around the deep basins of the Baltic Sea.
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  • 17
    Publication Date: 2022-04-06
    Description: A suite of oxygenated volatile organic compounds (OVOCs – acetaldehyde, acetone, propanal, butanal and butanone) were measured concurrently in the surface water and atmosphere of the South China Sea and Sulu Sea in November 2011. A strong correlation was observed between all OVOC concentrations in the surface seawater along the entire cruise track, except for acetaldehyde, suggesting similar sources and sinks in the surface ocean. Additionally, several phytoplankton groups, such as haptophytes or pelagophytes, were also correlated to all OVOCs, indicating that phytoplankton may be an important source of marine OVOCs in the South China and Sulu seas. Humic- and protein-like fluorescent dissolved organic matter (FDOM) components seemed to be additional precursors for butanone and acetaldehyde. The measurement-inferred OVOC fluxes generally showed an uptake of atmospheric OVOCs by the ocean for all gases, except for butanal. A few important exceptions were found along the Borneo coast, where OVOC fluxes from the ocean to the atmosphere were inferred. The atmospheric OVOC mixing ratios over the northern coast of Borneo were relatively high compared with literature values, suggesting that this coastal region is a local hotspot for atmospheric OVOCs. The calculated amount of OVOCs entrained into the ocean seemed to be an important source of OVOCs to the surface ocean. When the fluxes were out of the ocean, marine OVOCs were found to be enough to control the locally measured OVOC distribution in the atmosphere. Based on our model calculations, at least 0.4 ppb of marine-derived acetone and butanone can reach the upper troposphere, where they may have an important influence on hydrogen oxide radical formation over the western Pacific Ocean.
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  • 18
    Publication Date: 2020-02-06
    Description: This paper describes the recommended solar forcing dataset for CMIP6 and highlights changes with respect to CMIP5. The solar forcing is provided for radiative properties, namely total solar irradiance (TSI), solar spectral irradiance (SSI), and the F10.7 index as well as particle forcing, including geomagnetic indices Ap and Kp, and ionization rates to account for effects of solar protons, electrons, and galactic cosmic rays. This is the first time that a recommendation for solar-driven particle forcing has been provided for a CMIP exercise. The solar forcing datasets are provided at daily and monthly resolution separately for the CMIP6 preindustrial control, historical (1850–2014), and future (2015–2300) simulations. For the preindustrial control simulation, both constant and time-varying solar forcing components are provided, with the latter including variability on 11-year and shorter timescales but no long-term changes. For the future, we provide a realistic scenario of what solar behavior could be, as well as an additional extreme Maunder-minimum-like sensitivity scenario. This paper describes the forcing datasets and also provides detailed recommendations as to their implementation in current climate models. For the historical simulations, the TSI and SSI time series are defined as the average of two solar irradiance models that are adapted to CMIP6 needs: an empirical one (NRLTSI2–NRLSSI2) and a semi-empirical one (SATIRE). A new and lower TSI value is recommended: the contemporary solar-cycle average is now 1361.0 W m−2. The slight negative trend in TSI over the three most recent solar cycles in the CMIP6 dataset leads to only a small global radiative forcing of −0.04 W m−2. In the 200–400 nm wavelength range, which is important for ozone photochemistry, the CMIP6 solar forcing dataset shows a larger solar-cycle variability contribution to TSI than in CMIP5 (50 % compared to 35 %). We compare the climatic effects of the CMIP6 solar forcing dataset to its CMIP5 predecessor by using time-slice experiments of two chemistry–climate models and a reference radiative transfer model. The differences in the long-term mean SSI in the CMIP6 dataset, compared to CMIP5, impact on climatological stratospheric conditions (lower shortwave heating rates of −0.35 K day−1 at the stratopause), cooler stratospheric temperatures (−1.5 K in the upper stratosphere), lower ozone abundances in the lower stratosphere (−3 %), and higher ozone abundances (+1.5 % in the upper stratosphere and lower mesosphere). Between the maximum and minimum phases of the 11-year solar cycle, there is an increase in shortwave heating rates (+0.2 K day−1 at the stratopause), temperatures ( ∼  1 K at the stratopause), and ozone (+2.5 % in the upper stratosphere) in the tropical upper stratosphere using the CMIP6 forcing dataset. This solar-cycle response is slightly larger, but not statistically significantly different from that for the CMIP5 forcing dataset. CMIP6 models with a well-resolved shortwave radiation scheme are encouraged to prescribe SSI changes and include solar-induced stratospheric ozone variations, in order to better represent solar climate variability compared to models that only prescribe TSI and/or exclude the solar-ozone response. We show that monthly-mean solar-induced ozone variations are implicitly included in the SPARC/CCMI CMIP6 Ozone Database for historical simulations, which is derived from transient chemistry–climate model simulations and has been developed for climate models that do not calculate ozone interactively. CMIP6 models without chemistry that perform a preindustrial control simulation with time-varying solar forcing will need to use a modified version of the SPARC/CCMI Ozone Database that includes solar variability. CMIP6 models with interactive chemistry are also encouraged to use the particle forcing datasets, which will allow the potential long-term effects of particles to be addressed for the first time. The consideration of particle forcing has been shown to significantly improve the representation of reactive nitrogen and ozone variability in the polar middle atmosphere, eventually resulting in further improvements in the representation of solar climate variability in global models.
    Type: Article , PeerReviewed , info:eu-repo/semantics/article
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  • 19
    Publication Date: 2020-02-06
    Description: The pre-industrial millennium is among the periods selected by the Paleoclimate Model Intercomparison Project (PMIP) for experiments contributing to the sixth phase of the Coupled Model Intercomparison Project (CMIP6) and the fourth phase of the PMIP (PMIP4). The past1000 transient simulations serve to investigate the response to (mainly) natural forcing under background conditions not too different from today, and to discriminate between forced and internally generated variability on interannual to centennial timescales. This paper describes the motivation and the experimental set-ups for the PMIP4-CMIP6 past1000 simulations, and discusses the forcing agents orbital, solar, volcanic, and land use/land cover changes, and variations in greenhouse gas concentrations. The past1000 simulations covering the pre-industrial millennium from 850 Common Era (CE) to 1849 CE have to be complemented by historical simulations (1850 to 2014 CE) following the CMIP6 protocol. The external forcings for the past1000 experiments have been adapted to provide a seamless transition across these time periods. Protocols for the past1000 simulations have been divided into three tiers. A default forcing data set has been defined for the Tier 1 (the CMIP6 past1000) experiment. However, the PMIP community has maintained the flexibility to conduct coordinated sensitivity experiments to explore uncertainty in forcing reconstructions as well as parameter uncertainty in dedicated Tier 2 simulations. Additional experiments (Tier 3) are defined to foster collaborative model experiments focusing on the early instrumental period and to extend the temporal range and the scope of the simulations. This paper outlines current and future research foci and common analyses for collaborative work between the PMIP and the observational communities (reconstructions, instrumental data).
    Type: Article , PeerReviewed
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  • 20
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    Copernicus Publications (EGU)
    In:  Earth System Science Data, 9 . pp. 809-831.
    Publication Date: 2020-02-06
    Description: The injection of sulphur into the stratosphere by explosive volcanic eruptions is the cause of significant climate variability. Based on sulphate records from a suite of ice cores from Greenland and Antarctica, the eVolv2k database includes estimates of the magnitudes and approximate source latitudes of major volcanic stratospheric sulphur injection (VSSI) events from 500 BCE to 1900 CE, constituting an update of prior reconstructions and an extension of the record by 1000 years. The VSSI estimates incorporate improvements to the ice core records in terms of synchronization and dating, refinements to the methods used to estimate VSSI from ice core records, and includes first estimates of the random uncertainties in VSSI values. VSSI estimates for many of the largest eruptions, including Samalas (1257), Tambora (1815) and Laki (1783) are within 10% of prior estimates. A number of strong events are included in eVolv2k which are largely underestimated or not included in earlier VSSI reconstructions, including events in 540, 574, 682 and 1108 CE. The long term annual mean VSSI from major volcanic eruptions is estimated to be ∼ 0.5 Tg [S] yr−1, ∼ 50 % greater than a prior reconstruction, due to the identification of more events and an increase in the magnitude of many intermediate events. A long-term, latitudinally and monthly resolved stratospheric aerosol optical depth (SAOD) time series is reconstructed from the eVolv2k VSSI estimates, and the resulting global mean SAOD is found to be similar (within 33%) to a prior reconstruction for most of the largest eruptions. The long-term (500 BCE–900 CE) average global mean SAOD estimated from the eVolv2k VSSI estimates and including a constant "background" injection of stratospheric sulphur is ∼ 0.014, 30 % greater than a prior reconstruction. These new long-term reconstructions of past VSSI and SAOD variability give context to recent volcanic forcing, suggesting that the 20th century was a period of somewhat weaker than average volcanic forcing, with current best estimates of 20th century mean VSSI and SAOD values being 25 and 14 % less, respectively, than the mean of the 500 BCE to 1900 CE period. The reconstructed VSSI and SAOD data are available at https://doi.org/10.1594/WDCC/eVolv2k_v2〉.
    Type: Article , PeerReviewed
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