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.2010 Apr 13;107(15):6652-7.
doi: 10.1073/pnas.0908905107. Epub 2009 Dec 23.

Carbohydrate-like composition of submicron atmospheric particles and their production from ocean bubble bursting

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Carbohydrate-like composition of submicron atmospheric particles and their production from ocean bubble bursting

Lynn M Russell et al. Proc Natl Acad Sci U S A..

Abstract

Oceans cover over two-thirds of the Earth's surface, and the particles emitted to the atmosphere by waves breaking on sea surfaces provide an important contribution to the planetary albedo. During the International Chemistry Experiment in the Arctic LOwer Troposphere (ICEALOT) cruise on the R/V Knorr in March and April of 2008, organic mass accounted for 15-47% of the submicron particle mass in the air masses sampled over the North Atlantic and Arctic Oceans. A majority of this organic component (0.1-0.4 microm(-3)) consisted of organic hydroxyl (including polyol and other alcohol) groups characteristic of saccharides, similar to biogenic carbohydrates found in seawater. The large fraction of organic hydroxyl groups measured during ICEALOT in submicron atmospheric aerosol exceeded those measured in most previous campaigns but were similar to particles in marine air masses in the open ocean (Southeast Pacific Ocean) and coastal sites at northern Alaska (Barrow) and northeastern North America (Appledore Island and Chebogue Point). The ocean-derived organic hydroxyl mass concentration during ICEALOT correlated strongly to submicron Na concentration and wind speed. The observed submicron particle ratios of marine organic mass to Na were enriched by factors of approximately 10(2)-approximately 10(3) over reported sea surface organic to Na ratios, suggesting that the surface-controlled process of film bursting is influenced by the dissolved organic components present in the sea surface microlayer. Both marine organic components and Na increased with increasing number mean diameter of the accumulation mode, suggesting a possible link between organic components in the ocean surface and aerosol-cloud interactions.

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Conflict of interest statement

The authors declare no conflict of interest.

Figures

Fig. 1.
Fig. 1.
Contribution of OM1sea to OM1 (solid bars, bottom axis) for the Arctic, North Atlantic, and Other samples as well as the entire ICEALOT campaign, with project averages for Chebogue Point (ICARTT), VOCALS-REx, Barrow (2008), and Appledore Island (ICARTT) shown below. For the ICEALOT sectors of Arctic (dark blue), North Atlantic (chartreuse), and Other (gray), the middle bar shows the contribution of OM1sea (at left, cross-hatched) and submicron NaCl (at right, vertical lines) as mass fractions of PM1 (bottom axis) and the top bar (with diagonal lines) shows OM1sea concentration (top axis). Pie charts at right show the average FTIR functional group composition for each project and sector, where colors indicate organic hydroxyl (hot pink), alkane (blue), carboxylic acid (green), amine (orange), nonacidic carbonyl (teal), and organosulfate (yellow) groups as fractions of OM1, as shown in the legend.
Fig. 2.
Fig. 2.
Dependence of concentration of FTIR organic hydroxyl group concentration on (A) Na1 concentration (r = 0.74 for North Atlantic; r = 0.89 for Arctic; r = 0.30 for all), (B) wind speed (r = 0.89 for North Atlantic; r = 0.70 for Arctic; r = 0.26 for all), and dependence of concentration of PMF marine factor OM1sea on (C) Na1 concentration (r = 0.78 for North Atlantic; r = 0.91 for Arctic; r = 0.51 for all), (D) wind speed (r = 0.91 for North Atlantic; r = 0.90 for Arctic; r = 0.30 for all). Symbols and fit lines (with coefficients given inTable S3) are colored by sector as in Fig. 1; black line in (D) is the fit for both North Atlantic and Arctic sectors together, as given in Eq. [1].
Fig. 3.
Fig. 3.
FTIR spectra of (A) PMF-based marine factors for ICEALOT, VOCALS-REx, Barrow (winter), Chebogue Point (ICARTT), and Appledore Island (ICARTT) and (B) selected reference standards for saccharides as listed. The pie charts in (A) show the average composition of each of the marine factor FTIR spectra shown.
Fig. 4.
Fig. 4.
ICEALOT regional maps of potential source contribution functions for (A) organic hydroxyl group mass fractions of OM1 and (B) OM1sea/OM1. The colored lines show the cruise track, with colors indicating air mass sectors as in Fig. 1. The high probability potential source regions are colored dark red with lower probabilities in yellow. The pink diamond markers represent the locations of particles sampled for STXM-NEXAFS and EDX-SEM analysis shown in Fig. 5.
Fig. 5.
Fig. 5.
SEM-EDX spectra and images and STXM-NEXAFS C and K images of individual particles from ICEALOT and VOCALS-REx, illustrating organic coatings on crystallized NaCl. From left to right, each row shows “EDX” spectra, with absorption lines for C, O, N, Na (blue), Mg, Si (not shown because of substrate interference), S, primary Cl (blue), and secondary Cl; “SEM” image, with red box showing the region over which the EDX spectrum was averaged; “Pre-edge” of C by STXM-NEXAFS showing the particle regions that absorb before the C edge, which includes most atoms other than C; “Potassium” of STXM-NEXAFS showing the K containing particle regions; “Total Carbon” of STXM-NEXAFS showing the C-containing regions; “Alcohol” of STXM-NEXAFS (integrated from 289.3–289.5 eV) showing the organic hydroxyl containing regions. The particles shown in (A) and (B) are sampled during an unassigned time at the south end of the Arctic samples while the ship was north of Iceland, indicated by the marker in Fig. 4 at 71.5 N, 7.6 W on April 20, 2008 from 11:13 to 11:46; the particle in (C) was collected in Arctic air masses during ICEALOT indicated by the marker in Fig. 4 at 79.3 N, 9.2 E on April 15, 2008 from 13:26 to 13:36; the particle in (D) is collected during VOCALS-REx at 21.0 S, 82.9 W in a clean marine air mass on November 28, 2008 from 16:00 to 16:50.
Fig. 6.
Fig. 6.
Comparison of atmospheric and seawater ratios of organic carbon for the surface microlayer (SML) and OC1sea concentration in the marine boundary layer to Na1 concentration for Barrow Winter (purple), VOCALS-REx Southeast Pacific (salmon), ICEALOT North Atlantic (chartreuse), and ICEALOT Arctic (dark blue). SSW indicates subsurface water and MBL indicates marine boundary layer aerosol. The arrows show estimated MBL-SSW enrichment factors (EF) for each regional average aerosol OC1sea/Na1 based on measurements made previously in the same region for TOC/Na as listed in Table S4 [except for the Arctic where TOC is estimated based on Thurman et al. (29)], in which we note that seasonal differences are neglected: MBL-SSW EF are 174 (ICEALOT North Atlantic), 304 (ICEALOT Arctic), 160 (2008 Barrow summer), and 1843 (VOCALS SE Pacific). The cartoons on the right illustrate the differing amounts of POC and DOC that contribute to particle formation from bubble bursting in the Arctic and North Atlantic regions.
Fig. 7.
Fig. 7.
Dependence of D80 on (A) OM1sea and (B) Na1 for the Arctic (dark blue) and North Atlantic (chartreuse) air masses. Correlation coefficients for the linear fits (colored dashed lines) of D80 are 0.59 and 0.49 for OM1sea and 0.86 and 0.48 for Na1, both for the Arctic and North Atlantic, respectively. The solid black line in (A) shows the fit for both sectors, given in Eq. [2].
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