scholarly journals Marine submicron aerosol gradients, sources and sinks

2016 ◽  
Vol 16 (19) ◽  
pp. 12425-12439 ◽  
Author(s):  
Darius Ceburnis ◽  
Matteo Rinaldi ◽  
Jurgita Ovadnevaite ◽  
Giovanni Martucci ◽  
Lara Giulianelli ◽  
...  
Keyword(s):  
Organic Matter ◽  
Seasonal Pattern ◽  
Ammonium Oxalate ◽  
Methanesulfonic Acid ◽  
Sea Salt ◽  
Water Soluble ◽  
Sea Spray ◽  
Sampling System ◽  
Flux Footprint ◽  
Sources And Sinks

Abstract. Aerosol principal sources and sinks over eastern North Atlantic waters were studied through the deployment of an aerosol chemistry gradient sampling system. The chemical gradients of primary and secondary aerosol components – specifically, sea salt (SS), water-insoluble organic matter (WIOM), water-soluble organic matter (WSOM), nitrate, ammonium, oxalate, amines, methanesulfonic acid (MSA) and water-soluble organic nitrogen (WSON) – were examined in great detail. Sea salt fluxes were estimated by the boundary layer box model and ranged from 0.3 to 3.5 ng m−2 s−1 over the wind speed range of 5–12 m s−1 and compared well with the derived fluxes from existing sea salt source parameterisations. The observed seasonal pattern of sea salt gradients was mainly driven by wind stress in addition to the yet unquantified effect of marine OM modifying fractional contributions of SS and OM in sea spray. WIOM gradients were a complex combination of rising and waning biological activity, especially in the flux footprint area, and wind-driven primary sea spray production supporting the coupling of recently developed sea spray and marine OM parameterisations.

scholarly journals Marine submicron aerosol sources, sinks and chemical fluxes

2014 ◽  
Vol 14 (17) ◽  
pp. 23847-23889 ◽  
Author(s):  
D. Ceburnis ◽  
M. Rinaldi ◽  
J. Keane-Brennan ◽  
J. Ovadnevaite ◽  
G. Martucci ◽  
...  
Keyword(s):  
Wind Speed ◽  
Power Law ◽  
Salt Water ◽  
Ammonium Oxalate ◽  
Sea Salt ◽  
Water Soluble ◽  
Salt Flux ◽  
Sea Spray ◽  
Sampling System ◽  
Aerosol Sources

Abstract. The objectives of the study were to quantify seasonality in aerosol physico-chemical fluxes over NE Atlantic waters through the parallel deployment of micrometeorological eddy covariance flux system and an aerosol chemistry gradient sampling system. Fluxes of primary components (sea salt, water insoluble organic carbon and a combined sea spray) and secondary aerosol components (nitrate, ammonium, oxalate, amines, methanesulfonic acid and water soluble organic nitrogen) are presented in the context of seasonal marine aerosol sources and sinks. A strong power law relationship between fluxes and wind speed has been obtained not only for primary sea salt and sea spray, but also for secondary water soluble organic matter. The power law relationship between sea salt flux (FSSS) and 10 m height wind speed (U10) (FSSS=0.0011U103.15) compared very well with existing parameterisations using different approaches.

scholarly journals Linking variations in sea spray aerosol particle hygroscopicity to composition during two microcosm experiments

2016 ◽  
Vol 16 (14) ◽  
pp. 9003-9018 ◽  
Author(s):  
Sara D. Forestieri ◽  
Gavin C. Cornwell ◽  
Taylor M. Helgestad ◽  
Kathryn A. Moore ◽  
Christopher Lee ◽  
...  
Keyword(s):  
Organic Matter ◽  
Light Scattering ◽  
Time Lag ◽  
Sea Salt ◽  
Sea Spray ◽  
Phytoplankton Blooms ◽  
Chl A ◽  
Volume Fractions ◽  
Sea Spray Aerosol ◽  
Indoor And Outdoor

Abstract. The extent to which water uptake influences the light scattering ability of marine sea spray aerosol (SSA) particles depends critically on SSA chemical composition. The organic fraction of SSA can increase during phytoplankton blooms, decreasing the salt content and therefore the hygroscopicity of the particles. In this study, subsaturated hygroscopic growth factors at 85 % relative humidity (GF(85 %)) of predominately submicron SSA particles were quantified during two induced phytoplankton blooms in marine aerosol reference tanks (MARTs). One MART was illuminated with fluorescent lights and the other was illuminated with sunlight, referred to as the "indoor" and "outdoor" MARTs, respectively. Optically weighted GF(85 %) values for SSA particles were derived from measurements of light scattering and particle size distributions. The mean optically weighted SSA diameters were 530 and 570 nm for the indoor and outdoor MARTs, respectively. The GF(85 %) measurements were made concurrently with online particle composition measurements, including bulk composition (using an Aerodyne high-resolution aerosol mass spectrometer) and single particle (using an aerosol time-of-flight mass spectrometer) measurement, and a variety of water-composition measurements. During both microcosm experiments, the observed optically weighted GF(85 %) values were depressed substantially relative to pure inorganic sea salt by 5 to 15 %. There was also a time lag between GF(85 %) depression and the peak chlorophyll a (Chl a) concentrations by either 1 (indoor MART) or 3-to-6 (outdoor MART) days. The fraction of organic matter in the SSA particles generally increased after the Chl a peaked, also with a time lag, and ranged from about 0.25 to 0.5 by volume. The observed depression in the GF(85 %) values (relative to pure sea salt) is consistent with the large observed volume fractions of non-refractory organic matter (NR-OM) comprising the SSA. The GF(85 %) values exhibited a reasonable negative correlation with the SSA NR-OM volume fractions after the peak of the blooms (i.e., Chl a maxima); i.e., the GF(85 %) values generally decreased when the NR-OM volume fractions increased. The GF(85 %) vs. NR-OM volume fraction relationship was interpreted using the Zdanovskii–Stokes–Robinson (ZSR) mixing rule and used to estimate the GF(85 %) of the organic matter in the nascent SSA. The estimated pure NR-OM GF(85 %) values were 1.16 ± 0.09 and 1.23 ± 0.10 for the indoor and outdoor MARTS, respectively. These measurements demonstrate a clear relationship between SSA particle composition and the sensitivity of light scattering to variations in relative humidity. The implications of these observations to the direct climate effects of SSA particles are discussed.

scholarly journals A Two-Component Parameterization of Marine Ice Nucleating Particles Based on Seawater Biology and Sea Spray Aerosol Measurements in the Mediterranean Sea

2020 ◽  
Author(s):  
Jonathan V. Trueblood ◽  
Alesia Nicosia ◽  
Anja Engel ◽  
Birthe Zäncker ◽  
Matteo Rinaldi ◽  
...  
Keyword(s):  
Organic Matter ◽  
Mediterranean Sea ◽  
Biological Properties ◽  
Organic Content ◽  
Water Soluble ◽  
Sea Spray ◽  
Surface Microlayer ◽  
Natural Seawater ◽  
Order Of Magnitude ◽  
The Mediterranean

Abstract. Ice nucleating particles (INP) have a large impact on the climate-relevant properties of clouds over the oceans. Studies have shown that sea spray aerosols (SSA), produced upon bursting of bubbles at the ocean surface, can be an important source of marine INP, particularly during periods of enhanced biological productivity. Recent mesocosm experiments using natural seawater spiked with nutrients have revealed that marine INP are derived from two separate classes of organic matter in SSA. Despite this finding, existing parameterizations for marine INP abundance are based solely on single variables such as total organic carbon (TOC) or SSA surface area, which may mask specific trends in the separate classes of INPs. The goal of this paper is to improve the understanding of the connection between ocean biology and marine INP abundance by reporting results from a field study and proposing a new parameterization of marine INP that accounts for the two associated classes of organic matter. The PEACETIME cruise took place from May 10 to June 10, 2017 in the Mediterranean Sea. Throughout the cruise, INP concentrations in the surface microlayer (SML) and in SSA produced using a plunging aquarium apparatus were continuously monitored while surface seawater (SSW) and SML biological properties were measured in parallel. The organic content of artificially generated SSA was also evaluated. A dust wet deposition event that occurred during the cruise increased the INP concentrations measured in the SML by an order of magnitude, in line with increases of iron in the SML and bacterial abundances. Increases of INPs in marine SSA (INPSSA) were not observed before a delay of three days compared to increases in the SML, and are likely a result of a strong influence of bulk SSW INP for the temperatures investigated (T = −18 °C for SSA, T = −16 °C for SSW). Results confirmed that INPSSA are divided into two classes depending on their associated organic matter. Here we find that warm (T ≥ −22 °C) INPSSA concentrations are correlated with water soluble organic matter in the SSA, but also to SSW parameters (POCSSW INPSSW,−16 °C) while cold INPSSA (T 

scholarly journals Characteristics of methanesulfonic acid, non-sea-salt sulfate and organic carbon aerosols over the Amundsen Sea, Antarctica

2020 ◽  
Vol 20 (9) ◽  
pp. 5405-5424 ◽  
Author(s):  
Jinyoung Jung ◽  
Sang-Bum Hong ◽  
Meilian Chen ◽  
Jin Hur ◽  
Liping Jiao ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Southern Ocean ◽  
Methanesulfonic Acid ◽  
Austral Summer ◽  
Sea Salt ◽  
Water Soluble ◽  
Fluorescence Excitation ◽  
Amundsen Sea ◽  
Phaeocystis Antarctica ◽  
Seawater Samples

Abstract. To investigate the characteristics of particulate methanesulfonic acid (MSA(p)), non-sea-salt sulfate (nss SO42-) and organic carbon (OC) aerosols, aerosol and seawater samples were collected over the Southern Ocean (43–70∘ S) and the Amundsen Sea (70–75∘ S) during the ANA06B cruise conducted in the austral summer of 2016 aboard the Korean icebreaker IBR/V Araon. Over the Southern Ocean, the atmospheric MSA(p) concentration was low (0.10±0.002 µg m−3), whereas its concentration increased sharply up to 0.57 µg m−3 in the Amundsen Sea where Phaeocystis antarctica (P. antarctica), a producer of dimethylsulfide (DMS), was the dominant phytoplankton species. Unlike MSA(p), the mean nss SO42- concentration in the Amundsen Sea was comparable to that in the Southern Ocean. Water-soluble organic carbon (WSOC) concentrations over the Southern Ocean and the Amundsen Sea varied from 0.048 to 0.16 and 0.070 to 0.18 µgC m−3, with averages of 0.087±0.038 and 0.097±0.038 µgC m−3, respectively. For water-insoluble organic carbon (WIOC), its mean concentrations over the Southern Ocean and the Amundsen Sea were 0.25±0.13 and 0.26±0.10 µgC m−3, varying from 0.083 to 0.49 and 0.12 to 0.38 µgC m−3, respectively. WIOC was the dominant organic carbon species in both the Southern Ocean and the Amundsen Sea, accounting for 73 %–75 % of the total aerosol organic carbon. WSOC/Na+ and WIOC/Na+ ratios in the fine-mode aerosol particles were higher, especially in the Amundsen Sea where biological productivity was much higher than the Southern Ocean. The fluorescence properties of water-soluble organic aerosols investigated using a fluorescence excitation–emission matrix coupled with parallel factor analysis (EEM–PARAFAC) revealed that protein-like components were dominant in our marine aerosol samples, representing 69 %–91 % of the total intensity. Protein-like components also showed a significant positive relationship with the relative biomass of diatoms; however, they were negatively correlated with the relative biomass of P. antarctica. These results suggest that the protein-like component is most likely produced as a result of biological processes of diatoms in the Amundsen Sea.

An Aitken mode aerosol formation event in the high Arctic: evidence for aggregate breakup

2021 ◽  
Author(s):  
Michael Lawler ◽  
Eric Saltzman ◽  
Linn Karlsson ◽  
Paul Zieger ◽  
Matthew Salter ◽  
...  
Keyword(s):  
Atmospheric Transport ◽  
Methanesulfonic Acid ◽  
High Arctic ◽  
Sea Salt ◽  
Surface Energy Budget ◽  
Cloud Formation ◽  
Aerosol Size Distribution ◽  
Sea Spray ◽  
Aerosol Formation ◽  
Aitken Mode

<p>The summertime high Arctic is an extremely low-aerosol region, where even small inputs of particles can have significant impacts on cloud formation and therefore on the surface energy budget. The relative importance of new particle formation from gas phase precursors and primary sea spray production in this region remains uncertain, as does the role of atmospheric transport. We made direct, time-resolved composition measurements of Aitken mode (~20-60 nm diameter) aerosol over the high Arctic pack ice in August-September 2018, including during an intense Aitken mode formation event on August 30-31. The event particles contained both primary sea spray materials (sodium, potassium, and polysaccharide-like organics) and secondary components (non-sea-salt sulfate, methanesulfonic acid, non-sea-salt iodine, and secondary organics), most of which could be quantified on the basis of analytical standards. The composition is consistent with primary sea spray that had been atmospherically processed, and the aerosol size distribution dynamics imply the action of a process by which larger atmospheric particles or aggregates broke up to form smaller particles. Hypotheses to explain the results will be discussed.</p>

scholarly journals Sub-Antarctic marine aerosol: dominant contributions from biogenic sources

2013 ◽  
Vol 13 (17) ◽  
pp. 8669-8694 ◽  
Author(s):  
J. Schmale ◽  
J. Schneider ◽  
E. Nemitz ◽  
Y. S. Tang ◽  
U. Dragosits ◽  
...  
Keyword(s):  
Methanesulfonic Acid ◽  
Sea Salt ◽  
Submicron Particles ◽  
Sea Spray ◽  
Local Fauna ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass ◽  
Organic Factor ◽  
Sea Spray Aerosol ◽  
Highly Correlated

Abstract. Biogenic influences on the composition and characteristics of aerosol were investigated on Bird Island (54°00' S, 38°03' W) in the South Atlantic during November and December 2010. This remote marine environment is characterised by large seabird and seal colonies. The chemical composition of the submicron particles, measured by an aerosol mass spectrometer (AMS), was 21% non-sea-salt sulfate, 2% nitrate, 8% ammonium, 22% organics and 47% sea salt including sea salt sulfate. A new method to isolate the sea spray signature from the high-resolution AMS data was applied. Generally, the aerosol was found to be less acidic than in other marine environments due to the high availability of ammonia, from local fauna emissions. By positive matrix factorisation five different organic aerosol (OA) profiles could be isolated: an amino acid/amine factor (AA-OA, 18% of OA mass), a methanesulfonic acid OA factor (MSA-OA, 25%), a marine oxygenated OA factor (M-OOA, 41%), a sea spray OA fraction (SS-OA, 7%) and locally produced hydrocarbon-like OA (HOA, 9%). The AA-OA was dominant during the first two weeks of November and found to be related with the hatching of penguins in a nearby colony. This factor, rich in nitrogen (N : C ratio = 0.13), has implications for the biogeochemical cycling of nitrogen in the area as particulate matter is often transported over longer distances than gaseous N-rich compounds. The MSA-OA was mainly transported from more southerly latitudes where phytoplankton bloomed. The bloom was identified as one of three sources for particulate sulfate on Bird Island, next to sea salt sulfate and sulfate transported from South America. M-OOA was the dominant organic factor and found to be similar to marine OA observed at Mace Head, Ireland. An additional OA factor highly correlated with sea spray aerosol was identified (SS-OA). However, based on the available data the type of mixture, internal or external, could not be determined. Potassium was not associated with sea salt particles during 19% of the time, indicating the presence of biogenic particles in addition to the MSA-OA and AA-OA factors.

scholarly journals A two-component parameterization of marine ice-nucleating particles based on seawater biology and sea spray aerosol measurements in the Mediterranean Sea

2021 ◽  
Vol 21 (6) ◽  
pp. 4659-4676
Author(s):  
Jonathan V. Trueblood ◽  
Alessia Nicosia ◽  
Anja Engel ◽  
Birthe Zäncker ◽  
Matteo Rinaldi ◽  
...  
Keyword(s):  
Organic Matter ◽  
Organic Carbon ◽  
Mediterranean Sea ◽  
Water Soluble ◽  
Component Model ◽  
Sea Spray ◽  
Surface Microlayer ◽  
Model Based ◽  
Two Component ◽  
The Mediterranean

Abstract. Ice-nucleating particles (INPs) have a large impact on the climate-relevant properties of clouds over the oceans. Studies have shown that sea spray aerosols (SSAs), produced upon bursting of bubbles at the ocean surface, can be an important source of marine INPs, particularly during periods of enhanced biological productivity. Recent mesocosm experiments using natural seawater spiked with nutrients have revealed that marine INPs are derived from two separate classes of organic matter in SSAs. Despite this finding, existing parameterizations for marine INP abundance are based solely on single variables such as SSA organic carbon (OC) or SSA surface area, which may mask specific trends in the separate classes of INP. The goal of this paper is to improve the understanding of the connection between ocean biology and marine INP abundance by reporting results from a field study and proposing a new parameterization of marine INPs that accounts for the two associated classes of organic matter. The PEACETIME cruise took place from 10 May to 10 June 2017 in the Mediterranean Sea. Throughout the cruise, INP concentrations in the surface microlayer (INPSML) and in SSAs (INPSSA) produced using a plunging aquarium apparatus were continuously monitored while surface seawater (SSW) and SML biological properties were measured in parallel. The organic content of artificially generated SSAs was also evaluated. INPSML concentrations were found to be lower than those reported in the literature, presumably due to the oligotrophic nature of the Mediterranean Sea. A dust wet deposition event that occurred during the cruise increased the INP concentrations measured in the SML by an order of magnitude, in line with increases in iron in the SML and bacterial abundances. Increases in INPSSA were not observed until after a delay of 3 days compared to increases in the SML and are likely a result of a strong influence of bulk SSW INPs for the temperatures investigated (T=-18 ∘C for SSAs, T=-15 ∘C for SSW). Results confirmed that INPSSA are divided into two classes depending on their associated organic matter. Here we find that warm (T≥-22 ∘C) INPSSA concentrations are correlated with water-soluble organic matter (WSOC) in the SSAs, but also with SSW parameters (particulate organic carbon, POCSSW and INPSSW,-16C) while cold INPSSA (T<-22 ∘C) are correlated with SSA water-insoluble organic carbon (WIOC) and SML dissolved organic carbon (DOC) concentrations. A relationship was also found between cold INPSSA and SSW nano- and microphytoplankton cell abundances, indicating that these species might be a source of water-insoluble organic matter with surfactant properties and specific IN activities. Guided by these results, we formulated and tested multiple parameterizations for the abundance of INPs in marine SSAs, including a single-component model based on POCSSW and a two-component model based on SSA WIOC and OC. We also altered a previous model based on OCSSA content to account for oligotrophy of the Mediterranean Sea. We then compared this formulation with the previous models. This new parameterization should improve attempts to incorporate marine INP emissions into numerical models.

scholarly journals Dating of the GV7 East Antarctic ice core by high-resolution chemical records and focus on the accumulation rate variability in the last millennium

2021 ◽  
Vol 17 (5) ◽  
pp. 2073-2089
Author(s):  
Raffaello Nardin ◽  
Mirko Severi ◽  
Alessandra Amore ◽  
Silvia Becagli ◽  
Francois Burgay ◽  
...  
Keyword(s):  
Environmental Changes ◽  
18Th Century ◽  
Accumulation Rate ◽  
Seasonal Pattern ◽  
Ice Core ◽  
Methanesulfonic Acid ◽  
Snow Accumulation ◽  
Sea Salt ◽  
Last Millennium ◽  
Annual Layer

Abstract. Ice core dating is the first step for a correct interpretation of climatic and environmental changes. In this work, we release the dating of the uppermost 197 m of the 250 m deep GV7(B) ice core (drill site, 70∘41′ S, 158∘52′ E; 1950 m a.s.l. in Oates Land, East Antarctica) with a sub-annual resolution. Chemical records of NO3-, MSA (methanesulfonic acid), non-sea-salt SO42- (nssSO42-), sea-salt ions and water stable isotopes (δ18O) were studied as candidates for dating due to their seasonal pattern. Different procedures were tested but the nssSO42- record proved to be the most reliable on the short- and long-term scales, so it was chosen for annual layer counting along the whole ice core. The dating was constrained by using volcanic signatures from historically known events as tie points, thus providing an accurate age–depth relationship for the period 1179–2009 CE. The achievement of the complete age scale allowed us to calculate the annual mean accumulation rate throughout the analyzed 197 m of the core, yielding an annually resolved history of the snow accumulation on site in the last millennium. A small yet consistent rise in accumulation rate (Tr = 1.6, p<0.001) was found for the last 830 years starting around mid-18th century.

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