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Colin D Odowd - One of the best experts on this subject based on the ideXlab platform.

  • submicron ne atlantic Marine Aerosol chemical composition and abundance seasonal trends and air mass categorization
    Journal of Geophysical Research, 2014
    Co-Authors: Jurgita Ovadnevaite, Darius Ceburnis, Manuel Dallosto, H Berresheim, S Leinert, Manjula R Canagaratna, Simon Odoherty, Colin D Odowd
    Abstract:

    Three years of continuous Aerosol Mass Spectrometry measurements at the Mace Head Global Atmosphere Watch research station revealed seasonal patterns in the chemical composition of submicron NE Atlantic Marine Aerosol as well as distinct chemical signatures associated with Marine air masses of different origin (i.e., polar, Arctic, or tropical). Concentrations of secondary inorganic Aerosol species and both primary and secondary organic compounds were closely related to oceanic biological activity and ranged from low median mass concentrations during winter to high median values during summer as follows: 0.025–0.9 µg m−3 for nonsea-salt sulfate (nss-sulfate), 0.025–0.4 µg m−3 for organic matter, 0–0.09 µg m−3 for methanesulfonic acid (MSA). Sea-salt concentrations illustrated an opposite pattern with the highest median value being observed during winter (0.74 µg m−3) and lowest during summer (0.08 µg m−3). Maritime polar air masses typically featured the highest concentrations of sea salt and Marine organics, particularly enhanced under primary organic plumes during periods of high biological activity. MSA and nss-sulfate were more prominent in tropical air masses. The oxidation of organic matter increased with increasing ozone concentration and wintertime (low biological activity) organic matter displayed a different fragmentation pattern from that of summertime organic compounds.

  • is chlorophyll a the best surrogate for organic matter enrichment in submicron primary Marine Aerosol
    Journal of Geophysical Research, 2013
    Co-Authors: Matteo Rinaldi, Darius Ceburnis, Stefano Decesari, Sandro Fuzzi, Salvatore Marullo, Rosalia Santoleri, A Provenzale, Jost Von Hardenberg, Aditya Vaishya, Colin D Odowd
    Abstract:

    [1] Initial efforts toward developing a combined organic-inorganic sea spray source function parameterization for large-scale models made use of chlorophyll-a (Chl-a) and wind speed as input parameters to combine oceanic biology and atmospheric dynamics. These studies reported a modest correlation coefficient (0.55) between chlorophyll-a and organic matter (OM) enrichment in sea spray, suggesting that chlorophyll-a is only partially suitable for predicting organic enrichment. A reconstructed chlorophyll-a field of the North Atlantic Ocean from GlobColour reveals an improved correlation of 0.72 between the fractional mass contribution of organics in sea spray and chlorophyll-a concentration. A similar analysis, using colored dissolved and detrital organic material absorption and particulate organic carbon concentration, revealed slightly lower correlation coefficients (0.65 and 0.68). These results indicate that to date, chlorophyll-a is the best biological surrogate for predicting sea spray organic enrichment. In fact, considering the minimal difference between the correlation coefficients obtained with the three ocean color products, there is no reason to substitute chlorophyll-a, which is the most accurate parameter obtained from ocean color data, with other biological surrogates being generally affected by larger and less known errors. The observed time lag between chlorophyll-a concentration and organic matter enrichment in Aerosol suggests that biological processes in oceanic surface waters and their timescales should be considered when modeling the production of primary Marine organic Aerosol.

  • detecting high contributions of primary organic matter to Marine Aerosol a case study
    Geophysical Research Letters, 2011
    Co-Authors: Jurgita Ovadnevaite, Colin D Odowd, Darius Ceburnis, Manuel Dallosto, Douglas R Worsnop, H Berresheim
    Abstract:

    [1] Using on-line High-Resolution Aerosol Mass Spectrometry, we report submicron organic Marine Aerosol plume concentrations peaking at 3.8 μg m−3. These concentrations are far greater than previously determined by off-line techniques and can exceed typical terrestrial concentrations of organic Aerosol. The organic mass comprised 77% of the total submicron non-refractory mass and such plumes were associated with regions of high biological activity and moderately-high wind speeds over the N.E. Atlantic. High-resolution mass spectra analysis revealed a unique Marine organic Aerosol fingerprint, when compared to anthropogenic organic Aerosol, and in particular, anthropogenic hydrocarbons. 37% hydrocarbon and 63% oxygenated hydrocarbon speciation was observed for the organic mass, indicating that at least 37% of the organic mass is produced via primary sea-spray. The hydrocarbon and oxygenated hydrocarbon species were highly correlated (r > 0.99) suggesting a significant, if not dominant, fraction of the oxygenated component is also likely to be sea-spray in origin.

  • primary and secondary organic Marine Aerosol and oceanic biological activity recent results and new perspectives for future studies
    Advances in Meteorology, 2010
    Co-Authors: Matteo Rinaldi, Colin D Odowd, Darius Ceburnis, Stefano Decesari, C. Carbone, E. Finessi, Sandro Fuzzi, L Giulianelli, Maria Cristina Facchini
    Abstract:

    One of the most important natural Aerosol systems at the global level is Marine Aerosol that comprises both organic and inorganic components of primary and secondary origin. The present paper reviews some new results on primary and secondary organic Marine Aerosol, achieved during the EU project MAP (Marine Aerosol Production), comparing them with those reported in the recent literature. Marine Aerosol samples collected at the coastal site of Mace Head, Ireland, show a chemical composition trend that is influenced by the oceanic biological activity cycle, in agreement with other observations. Laboratory experiments show that sea-spray Aerosol from biologically active sea water can be highly enriched in organics, and the authors highlight the need for further studies on the atmospheric fate of such primary organics. With regard to the secondary fraction of organic Aerosol, the average chemical composition and molecular tracer (methanesulfonic-acid, amines) distribution could be successfully characterized by adopting a multitechnique analytical approach.

  • Marine Aerosol chemistry gradients elucidating primary and secondary processes and fluxes
    Geophysical Research Letters, 2008
    Co-Authors: Darius Ceburnis, Colin D Odowd, Stefano Decesari, Sandro Fuzzi, M C Facchini, L Emblico, Gerard Jennings, Jonas Sakalys
    Abstract:

    [1] Production mechanisms of Aerosol chemical species, in terms of primary and secondary processes, were studied using vertical concentration gradient measurements at the coastal research station in Mace Head, Ireland. Total gravimetric PM1.0 mass, sea salt and water insoluble organic carbon (WIOC) concentration profiles showed a net production at the surface (i.e. primary production), while nssSO4 and water soluble organic carbon (WSOC) concentration profiles showed a net removal at the surface. These observations indicate that WSOC was predominantly of secondary origin and that WIOC was predominantly of primary origin. Derived PM1 mass fluxes compared reasonably well with those previously obtained from an eddy covariance (EC) technique following a power law relationship with the wind speed (FPM1 = 0.000096*U4.23). For cases with clear primary organic mass fluxes in the flux footprint WIOM mass fluxes ranged between 0.16 and 1.02 ng m−2 s−1 and WIOM/sea salt mass ratio was 0.34–3.6, in good agreement with previous measurements at Mace Head.

Darius Ceburnis - One of the best experts on this subject based on the ideXlab platform.

  • Aerosol hygroscopicity and its link to chemical composition in the coastal atmosphere of Mace Head: Marine and continental air masses
    Atmospheric Chemistry and Physics, 2020
    Co-Authors: Jurgita Ovadnevaite, Kirsten N. Fossum, Chunshui Lin, Ru-jin Huang, Colin D. O'dowd, Darius Ceburnis
    Abstract:

    Abstract. Chemical composition and hygroscopicity closure of Marine Aerosol in high time resolution has not been achieved yet due to the difficulty involved in measuring the refractory sea-salt concentration in near-real time. In this study, attempts were made to achieve closure for Marine Aerosol based on a humidified tandem differential mobility analyser (HTDMA) and a high-resolution time-of-flight Aerosol mass spectrometer (AMS) for wintertime Aerosol at Mace Head, Ireland. The Aerosol hygroscopicity was examined as a growth factor (GF) at 90 % relative humidity (RH). The corresponding GFs of 35, 50, 75, 110 and 165 nm particles were 1.54±0.26 , 1.60±0.29 , 1.66±0.31 , 1.72±0.29 and 1.78±0.30 (mean  ±  standard deviation), respectively. Two contrasting air masses (continental and Marine) were selected to study the temporal variation in hygroscopicity; the results demonstrated a clear diurnal pattern in continental air masses, whereas no diurnal pattern was found in Marine air masses. In addition, wintertime Aerosol was observed to be largely externally mixed in both of the contrasting air masses. Concurrent high time resolution PM 1 (particulate matter  µ m) chemical composition data from combined AMS and MAAP measurements, comprising organic matter, non-sea-salt sulfate, nitrate, ammonium, sea salt and black carbon (BC), were used to predict Aerosol hygroscopicity with the Zdanovskii–Stokes–Robinson (ZSR) mixing rule. Overall, good agreement (an R2 value of 0.824 and a slope of 1.02) was found between the growth factor of 165 nm particles measured by the HTDMA (GF_HTDMA) and the growth factor derived from the AMS  +  MAAP bulk chemical composition (GF_AMS). Over 95 % of the estimated GF values exhibited less than a 10 % deviation for the whole dataset, and this deviation was mostly attributed to the neglected mixing state as a result of the bulk PM 1 composition.

  • stable isotopes measurements reveal dual carbon pools contributing to organic matter enrichment in Marine Aerosol
    Scientific Reports, 2016
    Co-Authors: Darius Ceburnis, Jurgita Ovadnevaite, Andrius Garbaras, Vidmantas Remeikis, M Claeys, J Sciare, Agne Masalaite, Willy Maenhaut, Dominique Baisnee
    Abstract:

    Stable carbon isotope ratios in Marine Aerosol collected over the Southern Indian Ocean revealed δ13C values ranging from −20.0‰ to −28.2‰. The isotope ratios exhibited a strong correlation with the fractional organic matter (OM) enrichment in sea spray Aerosol. The base-level isotope ratio of −20.0‰ is characteristic of an aged Dissolved Organic Matter (DOM) pool contributing a relatively homogeneous background level of DOM to oceanic waters. The range of isotope ratios, extending down to −28.2‰, is characteristic of more variable, stronger, and fresher Particulate Organic Matter (POM) pool driven by trophic level interactions. We present a conceptual dual-pool POM-DOM model which comprises a ‘young’ and variable POM pool which dominates enrichment in sea-spray and an ‘aged’ but invariant DOM pool which is, ultimately, an aged end-product of processed ‘fresh’ POM. This model is harmonious with the preferential enrichment of fresh colloidal and nano-gel lipid-like particulate matter in sea spray particles and the observed depleted δ13C ratio resulting from isotope equilibrium fractionation coupled with enhanced plankton photosynthesis in cold water (−2 °C to +8 °C). These results re-assert the hypothesis that OM enrichment in sea-spray is directly linked to primary production and, consequently, can have implications for climate-Aerosol-cloud feedback systems.

  • submicron ne atlantic Marine Aerosol chemical composition and abundance seasonal trends and air mass categorization
    Journal of Geophysical Research, 2014
    Co-Authors: Jurgita Ovadnevaite, Darius Ceburnis, Manuel Dallosto, H Berresheim, S Leinert, Manjula R Canagaratna, Simon Odoherty, Colin D Odowd
    Abstract:

    Three years of continuous Aerosol Mass Spectrometry measurements at the Mace Head Global Atmosphere Watch research station revealed seasonal patterns in the chemical composition of submicron NE Atlantic Marine Aerosol as well as distinct chemical signatures associated with Marine air masses of different origin (i.e., polar, Arctic, or tropical). Concentrations of secondary inorganic Aerosol species and both primary and secondary organic compounds were closely related to oceanic biological activity and ranged from low median mass concentrations during winter to high median values during summer as follows: 0.025–0.9 µg m−3 for nonsea-salt sulfate (nss-sulfate), 0.025–0.4 µg m−3 for organic matter, 0–0.09 µg m−3 for methanesulfonic acid (MSA). Sea-salt concentrations illustrated an opposite pattern with the highest median value being observed during winter (0.74 µg m−3) and lowest during summer (0.08 µg m−3). Maritime polar air masses typically featured the highest concentrations of sea salt and Marine organics, particularly enhanced under primary organic plumes during periods of high biological activity. MSA and nss-sulfate were more prominent in tropical air masses. The oxidation of organic matter increased with increasing ozone concentration and wintertime (low biological activity) organic matter displayed a different fragmentation pattern from that of summertime organic compounds.

  • is chlorophyll a the best surrogate for organic matter enrichment in submicron primary Marine Aerosol
    Journal of Geophysical Research, 2013
    Co-Authors: Matteo Rinaldi, Darius Ceburnis, Stefano Decesari, Sandro Fuzzi, Salvatore Marullo, Rosalia Santoleri, A Provenzale, Jost Von Hardenberg, Aditya Vaishya, Colin D Odowd
    Abstract:

    [1] Initial efforts toward developing a combined organic-inorganic sea spray source function parameterization for large-scale models made use of chlorophyll-a (Chl-a) and wind speed as input parameters to combine oceanic biology and atmospheric dynamics. These studies reported a modest correlation coefficient (0.55) between chlorophyll-a and organic matter (OM) enrichment in sea spray, suggesting that chlorophyll-a is only partially suitable for predicting organic enrichment. A reconstructed chlorophyll-a field of the North Atlantic Ocean from GlobColour reveals an improved correlation of 0.72 between the fractional mass contribution of organics in sea spray and chlorophyll-a concentration. A similar analysis, using colored dissolved and detrital organic material absorption and particulate organic carbon concentration, revealed slightly lower correlation coefficients (0.65 and 0.68). These results indicate that to date, chlorophyll-a is the best biological surrogate for predicting sea spray organic enrichment. In fact, considering the minimal difference between the correlation coefficients obtained with the three ocean color products, there is no reason to substitute chlorophyll-a, which is the most accurate parameter obtained from ocean color data, with other biological surrogates being generally affected by larger and less known errors. The observed time lag between chlorophyll-a concentration and organic matter enrichment in Aerosol suggests that biological processes in oceanic surface waters and their timescales should be considered when modeling the production of primary Marine organic Aerosol.

  • quantification of the carbonaceous matter origin in submicron Marine Aerosol by 13 c and 14 c isotope analysis
    Atmospheric Chemistry and Physics, 2011
    Co-Authors: Darius Ceburnis, Matteo Rinaldi, Andrius Garbaras, Soenke Szidat, S Fahrni, N Perron, Lukas Wacker, S Leinert, Vidmantas Remeikis
    Abstract:

    Abstract. Dual carbon isotope analysis of Marine Aerosol samples has been performed for the first time demonstrating a potential in organic matter apportionment between three principal sources: Marine, terrestrial (non-fossil) and fossil fuel due to unique isotopic signatures. The results presented here, utilising combinations of dual carbon isotope analysis, provides conclusive evidence of a dominant biogenic organic fraction to organic Aerosol over biologically active oceans. In particular, the NE Atlantic, which is also subjected to notable anthropogenic influences via pollution transport processes, was found to contain 80 % organic Aerosol matter of biogenic origin directly linked to plankton emissions. The remaining carbonaceous Aerosol was of terrestrial origin. By contrast, for polluted air advected out from Europe into the NE Atlantic, the source apportionment is 30 % Marine biogenic, 40 % fossil fuel, and 30 % continental non-fossil fuel. The dominant Marine organic Aerosol source in the atmosphere has significant implications for climate change feedback processes.

T S Bates - One of the best experts on this subject based on the ideXlab platform.

  • north atlantic Marine organic Aerosol characterized by novel offline thermal desorption mass spectrometry polysaccharides recalcitrant material and secondary organics
    Atmospheric Chemistry and Physics, 2020
    Co-Authors: Michael J Lawler, T S Bates, Lynn M Russell, Patricia K Quinn, S Lewis, D J Coffman, Lucia M Upchurch, Eric S Saltzman
    Abstract:

    Abstract. The composition of organic compounds in Marine Aerosols and the relative contributions of primary and secondary organic compounds remain uncertain. We report results from a novel approach to characterize and quantify organic components of the Marine Aerosol. Size-segregated discrete Aerosol filter samples were collected at sea in the North Atlantic from both ambient Aerosol and artificially generated primary sea spray over four cruises timed to capture the seasonal phytoplankton bloom dynamics. Samples were analyzed by Fourier transform infrared spectroscopy (FTIR), extracted into water, and analyzed by offline thermal desorption chemical ionization mass spectrometry (TDCIMS) and ion chromatography (IC). A positive matrix factorization (PMF) analysis identified several characteristic Aerosol components in the TDCIMS mass spectra. Among these is a “polysaccharide factor” representing about 10–30 % of the submicron organic Aerosol mass. An unquantified “recalcitrant factor” of highly thermally stable organics showed significant correlation with FTIR-measured alcohol groups, consistently the main organic functional group associated with sea spray Aerosol. We hypothesize that this factor represents recalcitrant dissolved organic matter in seawater. The recalcitrant factor showed little seasonal variability in its contribution to primary Marine Aerosol. The relative contribution of polysaccharides was highest in late spring and summer in the smallest particle size fraction characterized (< 180 nm).

  • seasonal variations in western north atlantic remote Marine Aerosol properties
    Journal of Geophysical Research, 2019
    Co-Authors: Patricia K Quinn, T S Bates, Richard H Moore, D J Coffman, Lucia Upchurch, James E Johnson, Luke D Ziemba
    Abstract:

    Author(s): Quinn, PK; Bates, TS; Coffman, DJ; Upchurch, L; Johnson, JE; Moore, R; Ziemba, L; Bell, TG; Saltzman, ES; Graff, J; Behrenfeld, MJ | Abstract: The impact of ocean ecosystems on Marine boundary layer Aerosols and clouds has been the subject of much research but remains uncertain. Five experiments were recently conducted in the western North Atlantic to assess if the seasonally recurring phytoplankton bloom affects Aerosol properties. These experiments include the second Western Atlantic Climate Study and four North Atlantic Aerosols and Marine Ecosystem Study cruises. Measurements of unheated and heated number size distributions, cloud condensation nucleus (CCN) concentrations, and Aerosol composition were used to identify primary and secondary Aerosol components that could be related to the state of the bloom. Only periods of clean Marine air, as defined by radon, particle number concentrations, Aerosol light absorption coefficient, and back trajectories, were included in the analysis. Nonvolatile material was found to be prevalent in the Aitken mode size range after heating to 230°, likely due to downward mixing from the free troposphere. CCN concentrations at 0.1% supersaturation were best correlated (r2 = 0.73) with accumulation mode nss SO4=. Sea spray Aerosol was only correlated with CCN during November when bloom accumulation had not yet occurred and dimethylsulfide concentrations were at a minimum. The fraction of CCN attributable to sea spray Aerosol was less than 20% during March, May/June, and September, indicating the limited contribution of sea spray Aerosol to the CCN population of the western North Atlantic atmosphere. The strongest link between the plankton bloom and Aerosol and cloud properties appears to be due to biogenic non-sea salt SO4=.

  • sources and composition of submicron organic mass in Marine Aerosol particles
    Journal of Geophysical Research, 2014
    Co-Authors: T S Bates, Amanda A Frossard, Lynn M Russell, Susannah M Burrows, Scott Elliott, Patricia K Quinn
    Abstract:

    The sources and composition of atmospheric Marine Aerosol particles (aMA) have been investigated with a range of physical and chemical measurements from open-ocean research cruises. This study uses the characteristic functional group composition (from Fourier transform infrared spectroscopy) of aMA from five ocean regions to show the following: (i) The organic functional group composition of aMA that can be identified as mainly atmospheric primary Marine (ocean derived) Aerosol particles (aPMA) is 65 ± 12% hydroxyl, 21 ± 9% alkane, 6 ± 6% amine, and 7 ± 8% carboxylic acid functional groups. Contributions from photochemical reactions add carboxylic acid groups (15%–25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal or continental emissions mix in alkane and carboxylic acid groups. (ii) The organic composition of aPMA is nearly identical to model-generated primary Marine Aerosol particles from bubbled seawater (gPMA, which has 55 ± 14% hydroxyl, 32 ± 14% alkane, and 13 ± 3% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied and the ratio of organic carbon to sodium (OC/Na+) in the gPMA remained nearly constant over a broad range of chlorophyll a concentrations, the gPMA alkane group fraction appeared to increase with chlorophyll a concentrations (r = 0.66). gPMA from productive seawater had a larger fraction of alkane functional groups (42 ± 9%) compared to gPMA from nonproductive seawater (22 ± 10%), perhaps due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater organic mass hydroxyl group peak location is closer to that of polysaccharides. This may result from the larger saccharides preferentially remaining in the seawater during gPMA and aPMA production.

  • light enhanced primary Marine Aerosol production from biologically productive seawater
    Geophysical Research Letters, 2014
    Co-Authors: Amanda A Frossard, Lynn M Russell, Patricia K Quinn, Michael S Long, William C Keene, David J Kieber, John R Maben, Joanna D Kinsey, T S Bates
    Abstract:

    Physical and biogeochemical processes in seawater controlling primary Marine Aerosol (PMA) production and composition are poorly understood and associated with large uncertainties in estimated fluxes into the atmosphere. PMA production was investigated in the biologically productive NE Pacific Ocean and in biologically productive and oligotrophic regions of the NW Atlantic Ocean. Physicochemical properties of model PMA, produced by aeration of fresh seawater under controlled conditions, were quantified. Diel variability in model PMA mass and number fluxes was observed in biologically productive waters, increasing following sunrise and decreasing to predawn levels overnight. Such variability was not seen in oligotrophic waters. During daytime, surfactant scavenging by aeration in the Aerosol generator without replenishing the seawater in the reservoir reduced the model PMA production in productive waters to nighttime levels but had no influence on production from oligotrophic waters. Results suggest bubble plume interactions with sunlight-mediated biogenic surfactants in productive seawater significantly enhanced model PMA production.

  • international global atmospheric chemistry igac project s first Aerosol characterization experiment ace 1 overview
    Journal of Geophysical Research, 1998
    Co-Authors: T S Bates, B J Huebert, J L Gras, Brian F Griffiths, Philip A Durkee
    Abstract:

    The southern hemisphere Marine Aerosol Characterization Experiment (ACE 1) was the first of a series of experiments that will quantify the chemical and physical processes controlling the evolution and properties of the atmospheric Aerosol relevant to radiative forcing and climate. The goals of this series of process studies are to reduce the overall uncertainty in the calculation of climate forcing by Aerosols and to understand the multiphase atmospheric chemical system sufficiently to be able to provide a prognostic analysis of future radiative forcing and climate response. ACE 1, which was conducted from November 15 to December 14, 1995, over the southwest Pacific Ocean, south of Australia, quantified the chemical, physical, radiative, and cloud nucleating properties and furthered our understanding of the processes controlling the Aerosol properties in this minimally polluted Marine atmosphere. The experiment involved the efforts of scientists from 45 research institutes in 11 countries.

Amanda A Frossard - One of the best experts on this subject based on the ideXlab platform.

  • oceanic efflux of ancient Marine dissolved organic carbon in primary Marine Aerosol
    Science Advances, 2019
    Co-Authors: Steven R Beaupre, Amanda A Frossard, Michael S Long, William C Keene, David J Kieber, John R Maben, Joanna D Kinsey, Yuting Zhu, Patrick Duplessis, R Y W Chang
    Abstract:

    Breaking waves produce bubble plumes that burst at the sea surface, injecting primary Marine Aerosol (PMA) highly enriched with Marine organic carbon (OC) into the atmosphere. It is widely assumed that this OC is modern, produced by present-day biological activity, even though nearly all Marine OC is thousands of years old, produced by biological activity long ago. We used natural abundance radiocarbon (14C) measurements to show that 19 to 40% of the OC associated with freshly produced PMA was refractory dissolved OC (RDOC). Globally, this process removes 2 to 20 Tg of RDOC from the oceans annually, comparable to other RDOC losses. This process represents a major removal pathway for old OC from the sea, with important implications for oceanic and atmospheric biogeochemistry, the global carbon cycle, and climate.

  • properties of seawater surfactants associated with primary Marine Aerosol particles produced by bursting bubbles at a model air sea interface
    Environmental Science & Technology, 2019
    Co-Authors: Amanda A Frossard, Michael S Long, John R Maben, Joanna D Kinsey, Yuting Zhu, Patrick Duplessis, R Y W Chang, Violaine Gerard, John Bisgrove, Steven R Beaupre
    Abstract:

    Surfactants account for minor fractions of total organic carbon in the ocean but can significantly influence the production of primary Marine Aerosol particles (PMA) at the sea surface via modulation of bubble surface tension. During September and October 2016, model PMA (mPMA) were produced from seawater by bursting bubbles at two biologically productive and two oligotrophic stations in the western North Atlantic Ocean. Total concentrations of surfactants extracted from mPMA and seawater were quantified and characterized via measurements of surface tension isotherms and critical micelle concentrations (CMCs). Surfactant CMCs in biologically productive seawater were lower than those in the oligotrophic seawater suggesting that surfactant mixtures in the two regions were chemically distinct. mPMA surfactants were enriched in all regions relative to those in the associated seawater. Surface tension isotherms indicate that mPMA surfactants were weaker than corresponding seawater surfactants. mPMA from biolog...

  • properties of seawater surfactants associated with primary Marine Aerosol particles produced by bursting bubbles at a model air sea interface
    Environmental Science & Technology, 2019
    Co-Authors: Amanda A Frossard, Michael S Long, John R Maben, Joanna D Kinsey, Yuting Zhu, Patrick Duplessis, R Y W Chang, Violaine Gerard, John Bisgrove, Steven R Beaupre
    Abstract:

    Surfactants account for minor fractions of total organic carbon in the ocean but can significantly influence the production of primary Marine Aerosol particles (PMA) at the sea surface via modulation of bubble surface tension. During September and October 2016, model PMA (mPMA) were produced from seawater by bursting bubbles at two biologically productive and two oligotrophic stations in the western North Atlantic Ocean. Total concentrations of surfactants extracted from mPMA and seawater were quantified and characterized via measurements of surface tension isotherms and critical micelle concentrations (CMCs). Surfactant CMCs in biologically productive seawater were lower than those in the oligotrophic seawater suggesting that surfactant mixtures in the two regions were chemically distinct. mPMA surfactants were enriched in all regions relative to those in the associated seawater. Surface tension isotherms indicate that mPMA surfactants were weaker than corresponding seawater surfactants. mPMA from biologically productive seawater contained higher concentrations of surfactants than those produced from oligotrophic seawater, supporting the hypothesis that seawater surfactant properties modulate mPMA surfactant concentrations. Diel variability in concentrations of seawater and mPMA surfactants in some regions is consistent with biological and/or photochemical processing. This work demonstrates direct links between surfactants in mPMA and those in the associated seawater.

  • factors that modulate properties of primary Marine Aerosol generated from ambient seawater on ships at sea
    Journal of Geophysical Research, 2017
    Co-Authors: William C Keene, Amanda A Frossard, Lynn M Russell, Michael S Long, David J Kieber, John R Maben, Joanna D Kinsey, Jeffrey S Reid
    Abstract:

    Model primary Marine Aerosol (mPMA) was produced by bubbling clean air through flowing natural seawater in a high-capacity generator deployed on ships in the eastern North Pacific and western North Atlantic Oceans. Physicochemical properties of seawater and mPMA were quantified to characterize factors that modulated production. Differences in surfactant organic matter (OM) and associated properties including surface tension sustained plumes with smaller bubble sizes, slower rise velocities, larger void fractions, and older surface ages in biologically productive relative to oligotrophic seawater. Production efficiencies for mPMA number (PEnum) and mass (PEmass) per unit air detrained from biologically productive seawater during daytime were greater and mass median diameters smaller than those in the same seawater at night and in oligotrophic seawater during day and night. PEmass decreased with increasing air detrainment rate suggesting that surface bubble rafts suppressed emission of jet droplets and associated mPMA mass. Relative to bubbles emitted at 60-cm depth, PEnum for bubbles emitted from 100-cm depth was approximately two times greater. mPMA OM enrichment factors (EFs) and mass fractions based on a coarse frit, fine frits, and a seawater jet exhibited similar size-dependent variability over a wide range in chlorophyll a concentrations. Results indicate that the physical production of PMA number and mass from the ocean surface varies systematically as interrelated functions of seawater type and, in biologically productive waters, time of day; bubble injection rate, depth, size, and surface age; and physical characteristics of the air-water interface whereas size-resolved OM EFs and mass fractions are relatively invariant.

  • primary Marine Aerosol cloud interactions off the coast of california
    Journal of Geophysical Research, 2015
    Co-Authors: Robin L Modini, Amanda A Frossard, Lars Ahlm, Lynn M Russell, C E Corrigan, G Roberts
    Abstract:

    Primary Marine Aerosol (PMA)-cloud interactions off the coast of California were investigated using observations of Marine Aerosol, cloud condensation nuclei (CCN), and stratocumulus clouds during the Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) and the Stratocumulus Observations of Los-Angeles Emissions Derived Aerosol-Droplets (SOLEDAD) studies. Based on recently reported measurements of PMA size distributions, a constrained lognormal-mode-fitting procedure was devised to isolate PMA number size distributions from total Aerosol size distributions and applied to E-PEACE measurements. During the 12 day E-PEACE cruise on the R/V Point Sur, PMA typically contributed less than 15% of total particle concentrations. PMA number concentrations averaged 12 cm^(−3) during a relatively calmer period (average wind speed 12 m/s^1) lasting 8 days, and 71 cm^(−3) during a period of higher wind speeds (average 16 m/s^1) lasting 5 days. On average, PMA contributed less than 10% of total CCN at supersaturations up to 0.9% during the calmer period; however, during the higher wind speed period, PMA comprised 5–63% of CCN (average 16–28%) at supersaturations less than 0.3%. Sea salt was measured directly in the dried residuals of cloud droplets during the SOLEDAD study. The mass fractions of sea salt in the residuals averaged 12 to 24% during three cloud events. Comparing the Marine stratocumulus clouds sampled in the two campaigns, measured peak supersaturations were 0.2 ± 0.04% during E-PEACE and 0.05–0.1% during SOLEDAD. The available measurements show that cloud droplet number concentrations increased with >100 nm particles in E-PEACE but decreased in the three SOLEDAD cloud events.

Michael S Long - One of the best experts on this subject based on the ideXlab platform.

  • oceanic efflux of ancient Marine dissolved organic carbon in primary Marine Aerosol
    Science Advances, 2019
    Co-Authors: Steven R Beaupre, Amanda A Frossard, Michael S Long, William C Keene, David J Kieber, John R Maben, Joanna D Kinsey, Yuting Zhu, Patrick Duplessis, R Y W Chang
    Abstract:

    Breaking waves produce bubble plumes that burst at the sea surface, injecting primary Marine Aerosol (PMA) highly enriched with Marine organic carbon (OC) into the atmosphere. It is widely assumed that this OC is modern, produced by present-day biological activity, even though nearly all Marine OC is thousands of years old, produced by biological activity long ago. We used natural abundance radiocarbon (14C) measurements to show that 19 to 40% of the OC associated with freshly produced PMA was refractory dissolved OC (RDOC). Globally, this process removes 2 to 20 Tg of RDOC from the oceans annually, comparable to other RDOC losses. This process represents a major removal pathway for old OC from the sea, with important implications for oceanic and atmospheric biogeochemistry, the global carbon cycle, and climate.

  • properties of seawater surfactants associated with primary Marine Aerosol particles produced by bursting bubbles at a model air sea interface
    Environmental Science & Technology, 2019
    Co-Authors: Amanda A Frossard, Michael S Long, John R Maben, Joanna D Kinsey, Yuting Zhu, Patrick Duplessis, R Y W Chang, Violaine Gerard, John Bisgrove, Steven R Beaupre
    Abstract:

    Surfactants account for minor fractions of total organic carbon in the ocean but can significantly influence the production of primary Marine Aerosol particles (PMA) at the sea surface via modulation of bubble surface tension. During September and October 2016, model PMA (mPMA) were produced from seawater by bursting bubbles at two biologically productive and two oligotrophic stations in the western North Atlantic Ocean. Total concentrations of surfactants extracted from mPMA and seawater were quantified and characterized via measurements of surface tension isotherms and critical micelle concentrations (CMCs). Surfactant CMCs in biologically productive seawater were lower than those in the oligotrophic seawater suggesting that surfactant mixtures in the two regions were chemically distinct. mPMA surfactants were enriched in all regions relative to those in the associated seawater. Surface tension isotherms indicate that mPMA surfactants were weaker than corresponding seawater surfactants. mPMA from biolog...

  • properties of seawater surfactants associated with primary Marine Aerosol particles produced by bursting bubbles at a model air sea interface
    Environmental Science & Technology, 2019
    Co-Authors: Amanda A Frossard, Michael S Long, John R Maben, Joanna D Kinsey, Yuting Zhu, Patrick Duplessis, R Y W Chang, Violaine Gerard, John Bisgrove, Steven R Beaupre
    Abstract:

    Surfactants account for minor fractions of total organic carbon in the ocean but can significantly influence the production of primary Marine Aerosol particles (PMA) at the sea surface via modulation of bubble surface tension. During September and October 2016, model PMA (mPMA) were produced from seawater by bursting bubbles at two biologically productive and two oligotrophic stations in the western North Atlantic Ocean. Total concentrations of surfactants extracted from mPMA and seawater were quantified and characterized via measurements of surface tension isotherms and critical micelle concentrations (CMCs). Surfactant CMCs in biologically productive seawater were lower than those in the oligotrophic seawater suggesting that surfactant mixtures in the two regions were chemically distinct. mPMA surfactants were enriched in all regions relative to those in the associated seawater. Surface tension isotherms indicate that mPMA surfactants were weaker than corresponding seawater surfactants. mPMA from biologically productive seawater contained higher concentrations of surfactants than those produced from oligotrophic seawater, supporting the hypothesis that seawater surfactant properties modulate mPMA surfactant concentrations. Diel variability in concentrations of seawater and mPMA surfactants in some regions is consistent with biological and/or photochemical processing. This work demonstrates direct links between surfactants in mPMA and those in the associated seawater.

  • factors that modulate properties of primary Marine Aerosol generated from ambient seawater on ships at sea
    Journal of Geophysical Research, 2017
    Co-Authors: William C Keene, Amanda A Frossard, Lynn M Russell, Michael S Long, David J Kieber, John R Maben, Joanna D Kinsey, Jeffrey S Reid
    Abstract:

    Model primary Marine Aerosol (mPMA) was produced by bubbling clean air through flowing natural seawater in a high-capacity generator deployed on ships in the eastern North Pacific and western North Atlantic Oceans. Physicochemical properties of seawater and mPMA were quantified to characterize factors that modulated production. Differences in surfactant organic matter (OM) and associated properties including surface tension sustained plumes with smaller bubble sizes, slower rise velocities, larger void fractions, and older surface ages in biologically productive relative to oligotrophic seawater. Production efficiencies for mPMA number (PEnum) and mass (PEmass) per unit air detrained from biologically productive seawater during daytime were greater and mass median diameters smaller than those in the same seawater at night and in oligotrophic seawater during day and night. PEmass decreased with increasing air detrainment rate suggesting that surface bubble rafts suppressed emission of jet droplets and associated mPMA mass. Relative to bubbles emitted at 60-cm depth, PEnum for bubbles emitted from 100-cm depth was approximately two times greater. mPMA OM enrichment factors (EFs) and mass fractions based on a coarse frit, fine frits, and a seawater jet exhibited similar size-dependent variability over a wide range in chlorophyll a concentrations. Results indicate that the physical production of PMA number and mass from the ocean surface varies systematically as interrelated functions of seawater type and, in biologically productive waters, time of day; bubble injection rate, depth, size, and surface age; and physical characteristics of the air-water interface whereas size-resolved OM EFs and mass fractions are relatively invariant.

  • light enhanced primary Marine Aerosol production from biologically productive seawater
    Geophysical Research Letters, 2014
    Co-Authors: Amanda A Frossard, Lynn M Russell, Patricia K Quinn, Michael S Long, William C Keene, David J Kieber, John R Maben, Joanna D Kinsey, T S Bates
    Abstract:

    Physical and biogeochemical processes in seawater controlling primary Marine Aerosol (PMA) production and composition are poorly understood and associated with large uncertainties in estimated fluxes into the atmosphere. PMA production was investigated in the biologically productive NE Pacific Ocean and in biologically productive and oligotrophic regions of the NW Atlantic Ocean. Physicochemical properties of model PMA, produced by aeration of fresh seawater under controlled conditions, were quantified. Diel variability in model PMA mass and number fluxes was observed in biologically productive waters, increasing following sunrise and decreasing to predawn levels overnight. Such variability was not seen in oligotrophic waters. During daytime, surfactant scavenging by aeration in the Aerosol generator without replenishing the seawater in the reservoir reduced the model PMA production in productive waters to nighttime levels but had no influence on production from oligotrophic waters. Results suggest bubble plume interactions with sunlight-mediated biogenic surfactants in productive seawater significantly enhanced model PMA production.