Molecular composition of the water‐soluble fraction of atmospheric carbonaceous aerosols collected during ACE‐Asia

Mader, Brian T.; Yu, Jian; Xu, Jinhui; Li, Q. F.; Wu, Wenbing; Flagan, Richard C.; Seinfeld, John H.

doi:10.1029/2003jd004105

Cited by 94 publications

(77 citation statements)

References 51 publications

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“…50% of the organics were found to be watersoluble (WSOC); other field studies have also reported WSOC concentrations of 30-70% of the total organics (Sempere and Kawamura 1994;Mader et al 2004).…”

Section: Estimation Of Molecular Weight Of Organic Components In Ambimentioning

confidence: 99%

Determination of Activity Coefficients of Semi-Volatile Organic Aerosols Using the Integrated Volume Method

Saleh

Khlystov

2009

Aerosol Science and Technology

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We demonstrate the use of the Integrated Volume Method (IVM) to estimate activity coefficients of semi-volatile organic compounds pertinent to ambient/atmospheric aerosols in binary mixtures. We generate binary solution aerosols with different mole fractions of individual components; for each mixture, we measure total change in aerosol volume upon heating from 25• C to 35• C, with the aerosols being at equilibrium in both states. The change in aerosol volume, or in other words, the partitioning between the particle phase and the gas phase, is used to determine activity coefficients of the compounds as a function of their mole fraction in the mixture. We demonstrate this method using the following four model systems. System 1: adipic acid-pimelic acid, which illustrates polar organic-polar organic interactions. Nonideal behavior was observed with activity coefficients around three at infinite dilution. System 2: adipic acid-dioctyl sebacate, which illustrates polar organic-non-polar organic interactions. The compounds in this experiment did not form a solution. System 3: adipic acid-ammonium sulfate, which illustrates polar organic-inorganic interactions. The compounds in this experiment did not form a solution. System 4: adipic acid-ambient extracts, which illustrates the potential use of the method to study partitioning behavior of individual components in a complex matrix approximating that of real ambient aerosol. The measured activity coefficients of adipic acid were less than unity for the tested range of mixing ratios, indicating suppression of volatility of this compound in ambient organic matrix.

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Section: Estimation Of Molecular Weight Of Organic Components In Ambimentioning

confidence: 99%

Determination of Activity Coefficients of Semi-Volatile Organic Aerosols Using the Integrated Volume Method

Saleh

Khlystov

2009

Aerosol Science and Technology

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“…Several types of L-amino acids have been identified in marine atmospheric aerosol samples ( Fig. 1), including, proline (PRO), serine (SER), glycine (GLY), alanine (ALA), valine (VAL), methionine (MET) and phenylalanine (PHE) (Mace et al, 2003a, b, c;Zhang and Anastasio, 2003;Malder et al, 2004;Wedyan and Preston, 2008). Over the central Arctic Ocean reaction products of L-methionine was suggested as being responsible for observed periods of new particle formation (Leck and Bigg, 1999).…”

Section: Introductionmentioning

confidence: 99%

“…The presence of secondary The DFAAs are shown in decreasing order of abundance (Malder et al, 2004): THR: threonine, GLU: glutamic acid, ASP: asparagine, CYS: cysteine, LYS: lysine, TYR: tyrosine, LEU: leucine, ILE: iso-leucine, HIS: histidine.…”

Section: Introductionmentioning

confidence: 99%

“…To study the cloud droplet condensational growth capacity of water-containing DFAAs representative for the remote marine atmosphere (Mopper and Zika, 1987;Spitzy, 1990;Mace et al, 2003a, b, c;Zhang and Anastasio, 2003;Malder et al, 2004;Wedyan and Preston, 2008), the structures and chemical properties of the following six L-amino acids (see Fig. 1) were investigated by the MD simulation technique: SER, GLY, ALA, VAL, MET and PHE.…”

Section: Introductionmentioning

confidence: 99%

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Cloud droplet activation mechanisms of amino acid aerosol particles: insight from molecular dynamics simulations

Hede

et al. 2013

Tellus B: Chemical and Physical Meteorology

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A B S T R A C T Atmospheric amino acids constitute a large fraction of water-soluble organic nitrogen compounds in aerosol particles, and have been confirmed as effective cloud condensation nuclei (CCN) materials in laboratory experiments. We present a molecular dynamics (MD) study of six amino acids with different structures and chemical properties that are relevant to the remote marine atmospheric aerosolÁcloud system, with the aim of investigating the detailed mechanism of their induced changes in surface activity and surface tension, which are important properties for cloud drop activation. Distributions and orientations of the amino acid molecules are studied; these L-amino acids are serine (SER), glycine (GLY), alanine (ALA), valine (VAL), methionine (MET) and phenylalanine (PHE) and are categorised as hydrophilic and amphiphilic according to their affinities to water. The results suggest that the presence of surface-concentrated amphiphilic amino acid molecules give rise to enhanced LennardÁJones repulsion, which in turn results in decreased surface tension of a planar interface and an increased surface tension of the spherical interface of droplets with diameters below 10 nm. The observed surface tension perturbation for the different amino acids under study not only serves as benchmark for future studies of more complex systems, but also shows that amphiphilic amino acids are surface active. The MD simulations used in this study reproduce experimental results of surface tension measurements for planar interfaces and the method is therefore applicable for spherical interfaces of nano-size for which experimental measurements are not possible to conduct.

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“…Organic matter can be 20-50 % of the total fine aerosol mass (Saxena and Hildemann, 1996;Putaud et al, 2004), and as high as 90 % over biomass burning regions during burning season (Andreae and Crutzen, 1997;Talbot et al, 1988Talbot et al, , 1990Artaxo et al, 1988Artaxo et al, , 1990Roberts et al, 2001;Bond et al, 2004). Between 45 and 75 % of this organic matter is watersoluble organic carbon (WSOC) and may therefore influence the hygroscopic growth behavior of atmospheric aerosols (Decesari et al, 2005;Saxena and Hildemann, 1996;Mader et al, 2004). This influence has been the subject of ongoing research during the past decade, though our knowledge is still limited (Kanakidou et al, 2005;Zhang et al, 2007;Hallquist et al, 2009).…”

mentioning

confidence: 99%

Measuring and modeling the hygroscopic growth of two humic substances in mixed aerosol particles of atmospheric relevance

Zamora

Jacobson

2013

Atmos. Chem. Phys.

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The hygroscopic growth of atmospheric particles affects atmospheric chemistry and Earth's climate. Water-soluble organic carbon (WSOC) constitutes a significant fraction of the dry submicron mass of atmospheric aerosols, thus affecting their water uptake properties. Although the WSOC fraction is comprised of many compounds, a set of model substances can be used to describe its behavior. For this study, mixtures of Nordic aquatic fulvic acid reference (NAFA) and Fluka humic acid (HA), with various combinations of inorganic salts (sodium chloride and ammonium sulfate) and other representative organic compounds (levoglucosan and succinic acid), were studied. We measured the equilibrium water vapor pressure over bulk solutions of these mixtures as a function of temperature and solute concentration. New water activity (a_w) parameterizations and hygroscopic growth curves at 25 °C were calculated from these data for particles of equivalent composition. We examined the effect of temperature on the water activity and found a maximum variation of 9% in the 0–30 °C range, and 2% in the 20–30 °C range. Five two-component mixtures were studied to understand the effect of adding a humic substance (HS), such as NAFA and HA, to an inorganic salt or a saccharide. The deliquescence point at 25 °C for HS-inorganic mixtures did not change significantly from that of the pure inorganic species. However, the hygroscopic growth of HA / inorganic mixtures was lower than that exhibited by the pure salt, in proportion to the added mass of HA. The addition of NAFA to a highly soluble solute (ammonium sulfate, sodium chloride or levoglucosan) in water had the same effect as the addition of HA to the inorganic species for most of the water activity range studied. Yet, the water uptake of these NAFA mixtures transitioned to match the growth of the pure salt or saccharide at high a_w values. The remaining four mixtures were based on chemical composition data for different aerosol types. As expected, the two solutions representing organic aerosols (40% HS/40% succinic acid/20% levoglucosan) showed lower water uptake than the two solutions representing biomass burning aerosols (25% HS/27% succinic acid/18% levoglucosan/30% ammonium sulfate). However, interactions in multicomponent solutions may be responsible for the large variation of the relative water uptake of identical mixtures containing different HSs above a water activity of 0.95. The ZSR (Zdanovskii, Stokes, and Robinson) model was able to predict reasonably well the hygroscopic growth of all the mixtures below a_w = 0.95, but produced large deviations for some multicomponent mixtures at higher values

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Molecular composition of the water‐soluble fraction of atmospheric carbonaceous aerosols collected during ACE‐Asia

Cited by 94 publications

References 51 publications

Determination of Activity Coefficients of Semi-Volatile Organic Aerosols Using the Integrated Volume Method

Determination of Activity Coefficients of Semi-Volatile Organic Aerosols Using the Integrated Volume Method

Cloud droplet activation mechanisms of amino acid aerosol particles: insight from molecular dynamics simulations

Measuring and modeling the hygroscopic growth of two humic substances in mixed aerosol particles of atmospheric relevance

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