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  • 1
    ISSN: 1573-0662
    Keywords: non-methane hydrocarbons ; ozone ; HO x ; CO ; NO x ; tropospheric chemistry ; global ; 3-d modeling ; upper troposphere
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract The impact of natural and anthropogenicnon-methane hydrocarbons (NMHC) on troposphericchemistry is investigated with the global,three-dimensional chemistry-transport model MOGUNTIA.This meteorologically simplified model allows theinclusion of a rather detailed scheme to describeNMHC oxidation chemistry. Comparing model resultscalculated with and without NMHC oxidation chemistryindicates that NMHC oxidation adds 40–60% to surfacecarbon monoxide (CO) levels over the continents andslightly less over the oceans. Free tropospheric COlevels increase by 30–60%. The overall yield of COfrom the NMHC mixture considered is calculated to beabout 0.4 CO per C atom. Organic nitrate formationduring NMHC oxidation, and their transport anddecomposition affect the global distribution of NO x and thereby O3 production. The impact of theshort-lived NMHC extends over the entire tropospheredue to the formation of longer-lived intermediateslike CO, and various carbonyl and carboxyl compounds.NMHC oxidation almost doubles the net photochemicalproduction of O3 in the troposphere and leads to20–80% higher O3 concentration inNO x -rich boundarylayers, with highest increases over and downwind ofthe industrial and biomass burning regions. Anincrease by 20–30% is calculated for the remotemarine atmosphere. At higher altitudes, smaller, butstill significant increases, in O3 concentrationsbetween 10 and 60% are calculated, maximizing in thetropics. NO from lightning also enhances the netchemical production of O3 by about 30%, leading to asimilar increase in the global mean OH radicalconcentration. NMHC oxidation decreases the OH radicalconcentrations in the continental boundary layer withlarge NMHC emissions by up to 20–60%. In the marineboundary layer (MBL) OH levels can increase in someregions by 10–20% depending on season and NO x levels.However, in most of the MBL OH will decrease by10–20% due to the increase in CO levels by NMHCoxidation chemistry. The large decreases especiallyover the continents strongly reduce the markedcontrasts in OHconcentrations between land and oceanwhich are calculated when only the backgroundchemistry is considered. In the middle troposphere, OHconcentrations are reduced by about 15%, although dueto the growth in CO. The overall effect of thesechanges on the tropospheric lifetime of CH4 is a 15%increase from 6.5 to 7.4 years. Biogenic hydrocarbonsdominate the impact of NMHC on global troposphericchemistry. Convection of hydrocarbon oxidationproducts: hydrogen peroxides and carbonyl compounds,especially acetone, is the main source of HO x in theupper troposphere. Convective transport and additionof NO from lightning are important for the O3 budgetin the free troposphere.
    Type of Medium: Electronic Resource
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  • 2
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    In:  Supplement to: Wong, Jenny Pui Shan; Tsagkaraki, Maria; Tsiodra, Irini; Mihalopoulos, Nikolaos; Violaki, Kalliopi; Kanakidou, Maria; Sciare, Jean; Nenes, Athanasios; Weber, Rodney J (2019): Atmospheric evolution of molecular-weight-separated brown carbon from biomass burning. Atmospheric Chemistry and Physics, 19(11), 7319-7334, https://doi.org/10.5194/acp-19-7319-2019
    Publication Date: 2023-01-13
    Description: Biomass burning is a major source of atmospheric brown carbon (BrC) and through its absorption of UV/VIS radiation, it can play an important role on the planetary radiative balance and atmospheric photochemistry. The considerable uncertainty of BrC impacts is associated with its poorly constrained sources, transformations and atmospheric lifetime. Here we report laboratory experiments that examined changes in the optical properties of the water-soluble BrC fraction of laboratory generated biomass burning particles from hardwood pyrolysis. Effects of direct UVB photolysis and OH oxidation in the aqueous phase on molecular weight-separated BrC were studied. Results indicated that the majority of low molecular weight (MW) BrC (〈 400 Da) was rapidly photobleached by both direct photolysis and OH oxidation on an atmospheric timescale of approximately 1 hour. High MW BrC (≥ 400 Da) underwent initial photoenhancement up to ~ 15 hours, followed by slow photobleaching over ~ 10 hours. The laboratory experiments were supported by observations from ambient BrC samples that were collected during the fire seasons in Greece. These samples, containing freshly emitted to aged biomass burning aerosol, were analyzed for both water and methanol soluble BrC. Consistent with the laboratory experiments, high MW BrC dominated the total light absorption at 365 nm for both methanol and water-soluble fractions of ambient samples with atmospheric transport times of 1 to 68 hours. These ambient observations indicate that overall, biomass burning BrC across all molecular weights have an atmospheric lifetime of 15 to 20 hours, consistent with estimates from previous field studies - although the BrC associated with the high MW fraction remains relatively stable and is responsible for light absorption properties of BrC throughout most of its atmospheric lifetime. For ambient samples of aged (〉 10 hours) biomass burning emissions, poor linear correlations were found between light absorptivity and levoglucosan, consistent with other studies suggesting a short atmospheric lifetime for levoglucosan. However, a much stronger correlation between light absorptivity and total hydrous sugars was observed, suggesting that they may serve as more robust tracers for aged biomass burning emissions. Overall, the results from this study suggest that robust model estimates of BrC radiative impacts require consideration of the atmospheric aging of BrC and the stability of high-MW BrC.
    Keywords: File format; File name; File size; Uniform resource locator/link to file
    Type: Dataset
    Format: text/tab-separated-values, 28 data points
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  • 3
    Publication Date: 2020-11-04
    Description: The global tropospheric budget of gaseous and particulate non-methane organic matter (OM) is re-examined to provide a holistic view of the role that OM plays in transporting the essential nutrients nitrogen and phosphorus to the ocean. A global 3-dimensional chemistry-transport model was used to construct the first global picture of atmospheric transport and deposition of the organic nitrogen (ON) and organic phosphorus (OP) that are associated with OM, focusing on the soluble fractions of these nutrients. Model simulations agree with observations within an order of magnitude. Depending on location, the observed water soluble ON fraction ranges from similar to 3% to 90% (median of similar to 35%) of total soluble N in rainwater; soluble OP ranges from similar to 20-83% (median of similar to 35%) of total soluble phosphorus. The simulations suggest that the global ON cycle has a strong anthropogenic component with similar to 45% of the overall atmospheric source (primary and secondary) associated with anthropogenic activities. In contrast, only 10% of atmospheric OP is emitted from human activities. The model-derived present-day soluble ON and OP deposition to the global ocean is estimated to be similar to 16 Tg-N/yr and similar to 0.35 Tg-P/yr respectively with an order of magnitude uncertainty. Of these amounts similar to 40% and similar to 6%, respectively, are associated with anthropogenic activities, and 33% and 90% are recycled oceanic materials. Therefore, anthropogenic emissions are having a greater impact on the ON cycle than the OP cycle; consequently increasing emissions may increase P-limitation in the oligotrophic regions of the world's ocean that rely on atmospheric deposition as an important nutrient source.
    Type: Article , PeerReviewed
    Format: text
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  • 4
    Publication Date: 2022-01-31
    Description: Anthropogenically-derived nitrogen input to the northern Indian Ocean has increased significantly in recent decades, based on both observational and model-derived estimates. This external nutrient source is supplied by atmospheric deposition and riverine fluxes, and has the potential to affect the vulnerable biogeochemical systems of the Arabian Sea and Bay of Bengal, influencing productivity and oceanic production of the greenhouse-gas nitrous-oxide (N 2 O). We summarize current estimates of this external nitrogen source to the northern Indian Ocean from observations and models, highlight implications for regional marine N 2 O emissions using model-based analyses, and make recommendations for measurement and model needs to improve current estimates and future predictions of this impact. Current observationally-derived estimates of deposition and riverine nitrogen inputs are limited by sparse measurements and uncertainties on accurate characterization of nitrogen species composition. Ocean model assessments of the impact of external nitrogen sources on regional marine N 2 O production in the northern Indian Ocean estimate potentially significant changes but also have large associated uncertainties. We recommend an integrated program of basin-wide measurements combined with high-resolution modeling and more detailed characterization of nitrogen-cycle process to address these uncertainties and improve current estimates and predictions.
    Type: Article , PeerReviewed
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  • 5
    Publication Date: 2024-02-07
    Description: The discovery of atmospheric micro(nano)plastic transport and ocean–atmosphere exchange points to a highly complex marine plastic cycle, with negative implications for human and ecosystem health. Yet, observations are currently limited. In this Perspective, we quantify the processes and fluxes of the marine-atmospheric micro(nano)plastic cycle, with the aim of highlighting the remaining unknowns in atmospheric micro(nano)plastic transport. Between 0.013 and 25 million metric tons per year of micro(nano)plastics are potentially being transported within the marine atmosphere and deposited in the oceans. However, the high uncertainty in these marine-atmospheric fluxes is related to data limitations and a lack of study intercomparability. To address the uncertainties and remaining knowledge gaps in the marine-atmospheric micro(nano)plastic cycle, we propose a future global marine-atmospheric micro(nano)plastic observation strategy, incorporating novel sampling methods and the creation of a comparable, harmonized and global data set. Together with long-term observations and intensive investigations, this strategy will help to define the trends in marine-atmospheric pollution and any responses to future policy and management actions.
    Type: Article , PeerReviewed
    Format: other
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  • 6
    Publication Date: 2022-10-27
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Pedrosa-Pamies, R., Parinos, C., Sanchez-Vidal, A., Calafat, A., Canals, M., Velaoras, D., Mihalopoulos, N., Kanakidou, M., Lampadariou, N., & Gogou, A. Atmospheric and oceanographic forcing impact particle flux composition and carbon sequestration in the eastern Mediterranean Sea: a three-year time-series study in the deep Ierapetra Basin. Frontiers in Earth Science, 9, (2021): 591948, https://doi.org/10.3389/feart.2021.591948.
    Description: Sinking particles are a critical conduit for the export of organic material from surface waters to the deep ocean. Despite their importance in oceanic carbon cycling, little is known about the biotic composition and seasonal variability of sinking particles reaching abyssal depths. Herein, sinking particle flux data, collected in the deep Ierapetra Basin for a three-year period (June 2010 to June 2013), have been examined at the light of atmospheric and oceanographic parameters and main mass components (lithogenic, opal, carbonates, nitrogen, and organic carbon), stable isotopes of particulate organic carbon (POC) and source-specific lipid biomarkers. Our aim is to improve the current understanding of the dynamics of particle fluxes and the linkages between atmospheric dynamics and ocean biogeochemistry shaping the export of organic matter in the deep Eastern Mediterranean Sea. Overall, particle fluxes showed seasonality and interannual variability over the studied period. POC fluxes peaked in spring April–May 2012 (12.2 mg m−2 d−1) related with extreme atmospheric forcing. Summer export was approximately fourfold higher than mean wintertime, fall and springtime (except for the episodic event of spring 2012), fueling efficient organic carbon sequestration. Lipid biomarkers indicate a high relative contribution of natural and anthropogenic, marine- and land-derived POC during both spring (April–May) and summer (June–July) reaching the deep-sea floor. Moreover, our results highlight that both seasonal and episodic pulses are crucial for POC export, while the coupling of extreme weather events and atmospheric deposition can trigger the influx of both marine labile carbon and anthropogenic compounds to the deep Levantine Sea. Finally, the comparison of time series data of sinking particulate flux with the corresponding biogeochemical parameters data previously reported for surface sediment samples from the deep-sea shed light on the benthic–pelagic coupling in the study area. Thus, this study underscores that accounting the seasonal and episodic pulses of organic carbon into the deep sea is critical in modeling the depth and intensity of natural and anthropogenic POC sequestration, and for a better understanding of the global carbon cycle.
    Description: This research was supported by the REDECO (CTM2008-04973-E/MAR) and PERSEUS (GA 287600) projects. We further acknowledge support by the projects PANACEA—‘PANhellenic infrastructure for Atmospheric Composition and climatE chAnge’ (MIS 5021516) and ENIRISST—‘Intelligent Research Infrastructure for Shipping, Supply Chain, Transport and Logistics’ (MIS 5027930), which are implemented under the Action “Reinforcement of the Research and Innovation Infrastructure,” funded by the Operational Program “Competitiveness, Entrepreneurship and Innovation” (NSRF 2014-2020) and co-financed by Greece and EU; and by the Action “National Νetwork on Climate Change and its Impacts - Climpact” which is implemented under the sub-project 3 of the project “Infrastructure of national research networks in the fields of Precision Medicine, Quantum Technology and Climate Change,” funded by the Public Investment Program of Greece, General Secretary of Research and Technology/Ministry of Development and Investments.” Researchers from GRC Geociències Marines benefited from a Grups de Recerca Consolidats grant (2017 SGR 315) by Generalitat de Catalunya autonomous government.
    Keywords: Sinking particle fluxes ; Carbon cycle ; Lipid biomarkers ; Atmospheric forcing ; Eastern mediterranean sea ; Surface sediment ; Deep ocean ; Particulate organic carbon
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 7
    Publication Date: 2022-11-03
    Description: The discovery of atmospheric micro(nano)plastic transport and ocean–atmosphere exchange points to a highly complex marine plastic cycle, with negative implications for human and ecosystem health. Yet, observations are currently limited. In this Perspective, we quantify the processes and fluxes of the marine-atmospheric micro(nano)plastic cycle, with the aim of highlighting the remaining unknowns in atmospheric micro(nano)plastic transport. Between 0.013 and 25 million metric tons per year of micro(nano)plastics are potentially being transported within the marine atmosphere and deposited in the oceans. However, the high uncertainty in these marine-atmospheric fluxes is related to data limitations and a lack of study intercomparability. To address the uncertainties and remaining knowledge gaps in the marine-atmospheric micro(nano)plastic cycle, we propose a future global marine-atmospheric micro(nano)plastic observation strategy, incorporating novel sampling methods and the creation of a comparable, harmonized and global data set. Together with long-term observations and intensive investigations, this strategy will help to define the trends in marine-atmospheric pollution and any responses to future policy and management actions.
    Repository Name: EPIC Alfred Wegener Institut
    Type: Article , isiRev
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