scholarly journals Contribution of particulate sulfate and organic carbon to cloud condensation nuclei in the marine atmosphere

1997 ◽  
Vol 24 (6) ◽  
pp. 655-658 ◽  
Author(s):  
Kiyoshi Matsumoto ◽  
Hiroshi Tanaka ◽  
Ippei Nagao ◽  
Yutaka Ishizaka
2021 ◽  
Vol 118 (42) ◽  
pp. e2110472118
Author(s):  
Gordon A. Novak ◽  
Charles H. Fite ◽  
Christopher D. Holmes ◽  
Patrick R. Veres ◽  
J. Andrew Neuman ◽  
...  

Oceans emit large quantities of dimethyl sulfide (DMS) to the marine atmosphere. The oxidation of DMS leads to the formation and growth of cloud condensation nuclei (CCN) with consequent effects on Earth’s radiation balance and climate. The quantitative assessment of the impact of DMS emissions on CCN concentrations necessitates a detailed description of the oxidation of DMS in the presence of existing aerosol particles and clouds. In the unpolluted marine atmosphere, DMS is efficiently oxidized to hydroperoxymethyl thioformate (HPMTF), a stable intermediate in the chemical trajectory toward sulfur dioxide (SO2) and ultimately sulfate aerosol. Using direct airborne flux measurements, we demonstrate that the irreversible loss of HPMTF to clouds in the marine boundary layer determines the HPMTF lifetime (τHPMTF < 2 h) and terminates DMS oxidation to SO2. When accounting for HPMTF cloud loss in a global chemical transport model, we show that SO2 production from DMS is reduced by 35% globally and near-surface (0 to 3 km) SO2 concentrations over the ocean are lowered by 24%. This large, previously unconsidered loss process for volatile sulfur accelerates the timescale for the conversion of DMS to sulfate while limiting new particle formation in the marine atmosphere and changing the dynamics of aerosol growth. This loss process potentially reduces the spatial scale over which DMS emissions contribute to aerosol production and growth and weakens the link between DMS emission and marine CCN production with subsequent implications for cloud formation, radiative forcing, and climate.


2020 ◽  
Vol 20 (15) ◽  
pp. 9153-9167 ◽  
Author(s):  
Mingfu Cai ◽  
Baoling Liang ◽  
Qibin Sun ◽  
Shengzhen Zhou ◽  
Xiaoyang Chen ◽  
...  

Abstract. Aerosol particles in marine atmosphere have been shown to significantly affect cloud formation, atmospheric optical properties, and climate change. However, high temporally and spatially resolved atmospheric measurements over the sea are currently sparse, limiting our understanding of aerosol properties in marine atmosphere. In this study, a ship-based cruise campaign was conducted over the northern South China Sea (SCS) region during summertime 2018. The chemical composition of non-refractory PM1 (NR-PM1), the particle number size distribution (PNSD), and size-resolved cloud condensation nuclei (CCN) activity were measured by a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) and the combination of a cloud condensation nuclei counter (CCNc) and a scanning mobility particle sizer (SMPS). Overall, aerosol particles exhibited a unimodal distribution centering at 60–80 nm and the chemical composition of the NR-PM1 was dominated by sulfate (∼ 46 %), which likely originated from anthropogenic emissions rather than dimethyl sulfide (DMS) oxidation. Two polluted episodes (P1 and P2) were observed, and both were characterized by high particle number concentrations (NCN) which originated from local emissions and from emissions in inland China via long-range transport. The concentrations of trace gases (i.e., O3, CO, NOx) and particles (NCN and NCCN at ss = 0.34 %) were elevated during P2 at the end of the campaign and decreased with offshore distance, further suggesting important impacts of anthropogenic emissions from the inland Pearl River Delta (PRD) region. Two relatively clean periods (C1 and C2) prior to and after tropical storm Bebinca were classified and the air was affected by air masses from the southwest and from the Indo-Chinese Peninsula, respectively. Chemical composition measurements showed an increase in organic mass fraction during P2 compared to C2; however, no obviously different κ values were obtained from the CCNc measurements, implying that the air masses carried pollutants from local sources during long-range transport. We report an average value of about 0.4 for the aerosol hygroscopicity parameter κ, which falls within the literature values (i.e., 0.2–1.0) for urban and remote marine atmosphere. In addition, our results showed that the CCN fraction (NCCN∕NCN, tot) and the κ values had no clear correlation either with the offshore distance or with concentrations of the particles. Our study highlights dynamical variations in particle properties and the impact of long-range transport from continental China and the Indo-Chinese Peninsula on the northern SCS region during summertime.


2008 ◽  
Vol 8 (11) ◽  
pp. 2933-2948 ◽  
Author(s):  
M. Kuwata ◽  
Y. Kondo ◽  
Y. Miyazaki ◽  
Y. Komazaki ◽  
J. H. Kim ◽  
...  

Abstract. We measured the number concentrations of cloud condensation nuclei (CCN) and the size distributions of CCN/CN (CN: condensation nuclei) ratios at supersaturations (SSs) of 0.097, 0.27, 0.58, and 0.97% at Jeju Island, Korea during March-April 2005. We made simultaneous measurements of aerosol inorganic ions, water-soluble organic carbon (WSOC), organic carbon (OC), and elemental carbon (EC) in PM2.5. The CCN/CN ratios increased with increasing particle diameter, and the diameter at CCN/CN=0.5 was defined as D50. D50 represents the activation dry diameter of atmospheric particles. The average D50 at SS=0.097% and 0.97% was 136±17 nm and 31±3 nm, respectively. The temporal variation of D50 at SS=0.097% was correlated with the mass fraction of water-soluble components (inorganic ions + WSOC), indicating that the temporal variation of CCN activity was mainly controlled by changes in the water-soluble components fraction. The critical dry diameter (Dcrit), which is the threshold dry diameter for CCN activation, was calculated from the observed aerosol chemical compositions by Köhler theory for comparison with D50. The D50 at SS=0.097% was correlated (r2=0.48) with calculated Dcrit, although Dcrit was larger than D50 by 20–29% on average. The systematic difference between D50 and Dcrit could be caused by the size dependence of the aerosol chemical compositions or surface tension lowering caused by the mixing of water-soluble organic compounds. This difference corresponds to a 27±14% uncertainty in the CCN number concentration estimated from the observed particle number size distribution.


2020 ◽  
Author(s):  
Mingfu Cai ◽  
Baoling Liang ◽  
Qibin Sun ◽  
Shengzhen Zhou ◽  
Bin Yuan ◽  
...  

Abstract. Aerosol particles in marine atmosphere have been shown to significantly affect cloud formation, atmospheric optical properties, and climate change. However, high temporal and spatial resolved atmospheric measurements over sea are currently sparse, limiting our understanding of aerosol properties in marine atmosphere. In this study, a ship-based cruise campaign was conducted over northern South China Sea (SCS) region (19°37′ N to 22°43′ N, 113°44′ E to 118°12′ E) during summertime 2018. Chemical compositions of the non-refractory PM1 (NR-PM1), particle number size distribution (PNSD) and size-resolved cloud condensation nuclei (CCN) activity (at supersaturation ss = 0.18 %, 0.34 %, and 0.59 %) were measured by a time-of-flight aerosol chemical speciation monitor (ToF-ACSM), and the combination of a cloud condensation nuclei counter (CCNc) and a scanning mobility particle sizer (SMPS), respectively. Overall, aerosol particles exhibited a unimodal distribution (centering at 60∼80 nm) and dominated by sulfate (~46 %) in the NR-PM1, similar to the characteristic of previously-reported background marine aerosols. Two polluted episodes were respectively observed at the beginning (P1, 6th–8th August) and at the end (P2, 25th–26th August) of the campaign and both were characterized by high particle number concentrations (NCN) which were shown to originate from local emissions or pollutants from long range transport. Two relatively clean periods (C1, 9th–10th and C2, 19th–21st August) prior to and after tropical storm Bebinca (11th–15th August) were also classified due to substantial removal of pollutants by strong winds and rainfalls accompanying with the storm. A value of about 0.4 for aerosol hygroscopicity parameter κ measured in this study falls in a range of values (i.e., 0.2–1.0) reported previously for urban atmosphere and for remote marine atmosphere. The concentrations of trace gases (i.e., O3, CO, NOX) and particles (NCN and NCCN at ss = 0.34 %) were elevated at the end of the campaign and decreased with the offshore distance, suggesting important impacts of anthropogenic emissions from the inland Pearl River Delta (PRD) region on the northern SCS. A good correlation between NOX concentration and NCN implies similar sources (e.g., heavy ship, traffic, and biomass burning) for NOx and particles. The results showed that the NCCN/NCN,tot and the κ values obtained from the CCNc measurement (ss = 0.34 %) had no clear correlation either with the offshore distance or with the concentrations of the particles. Back trajectory analysis showed that the air pollutants originated from local emissions and from inland China continent via long range transport during P1 and P2, respectively. In addition, the air was affected by air masses from southwest and from Indo-China Peninsula during the clean C1 and C2 periods respectively. Chemical composition measurements showed an increase of organic mass fraction and no obviously different κ values were obtained from CCN measurements during C2 and P2, implying that the air masses carried pollutants from local sources during long range transport from Indo-China Peninsula and from the inland China continent respectively during the above two periods. Our study highlights dynamical variations of particle properties and the impact of long range transport from the China continent and Indo-China Peninsula on the northern SCS region during summertime.


2007 ◽  
Vol 7 (6) ◽  
pp. 15805-15851 ◽  
Author(s):  
M. Kuwata ◽  
Y. Kondo ◽  
Y. Miyazaki ◽  
Y. Komazaki ◽  
J. H. Kim ◽  
...  

Abstract. We measured the number concentrations of cloud condensation nuclei (CCN) and the size distributions of CCN/CN (CN: condensation nuclei) ratios at supersaturations (SSs) of 0.097, 0.27, 0.58, and 0.97% at Jeju-Island, Korea during March-April 2005. Measurements of aerosol inorganic ions, water-soluble organic carbon (WSOC), organic carbon (OC), and elemental carbon (EC) in PM2.5 were simultaneously made. The CCN/CN ratios increased with increasing particle diameter, and the diameter at CCN/CN=0.5 was defined as D50. D50 represents the activation dry diameter of atmospheric particles. The average D50 at SS=0.097% and 0.97% was 136 nm and 31 nm, respectively. The temporal variation of D50 at SS=0.097% was correlated with the mass fraction of water-soluble components (inorganic ions + WSOC), indicating that the temporal variation of CCN activity was mainly controlled by changes in the water-soluble components fraction. The critical dry diameter (Dcrit), which is the threshold dry diameter for CCN activation, was calculated from the observed aerosol chemical compositions by Köhler theory for comparison with D50. The D50 at SS=0.097% was correlated (r2=0.48) with calculated Dcrit, although Dcrit were larger than D50 by 20–29% on average. The systematic difference between D50 and Dcrit could be caused by the size dependence of the aerosol chemical compositions or surface tension lowering caused by the mixing of water-soluble organic compounds. This difference corresponds to a 27±14% uncertainty in the CCN number concentration estimated from the observed particle number size distribution.


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