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1 Feature Article J. Aerosol Res.19 NOAA R/V Ronald H. Brown ACE-Asia Atmospheric Aerosol Study on NOAA R/V Ronald H. Brown during ACE-Asia Campaign Michihiro MOCHIDA and Kimitaka KAWAMURA Received March Accepted April Abstract As part of Aerosol Characterization ExperimentACE-Asia campaign, a comprehensive study was conducted from March to April on board NOAA R/V Ronald H. Brown over the North Pacific, the East China Sea and the Sea of Japan. More than research groups participated in this research cruise for the measurements of aerosol chemical, physical, and optical properties, as well as the measurements of precursor gases, seawater, and radiant flux. Authors research group conducted an aerosol study on the chemical speciation of organic compounds, including a series of dicarboxylic acids, fatty acids, and levoglucosan. The spatial distributions of oxygenated organic compounds over the western North Pacific clearly demonstrate that Asian outflow regulates the concentrations of organic aerosols in the marine atmosphere. Key Words ACE-Asia, Carbonaceous Particles, Transport Process, Oxygenated Organic Compounds. - Institute of Low Temperature Science, Hokkaido University N, W, Kita-ku, Sapporo - Aerosol Characterization ExperimentACE- Asia ACE-Asia NOAA Ronald H. Brown RHB INDOEXIndian Ocean Experiment RHB ACE-Asia ACE-Asia RHB, ACE-Asia

2 RHB ACE-Asia RHB ACE-Asia Overview Fig. 1 ACE-Asia RHB ACE-Asia RHB RHB CTwin OtterKing Air Terra/MISR van Fig. 2 RHB Fig. Cruise Track March April, a b Level FOCSLE DECKLevel Ship Van AI Van PMEL Van Lidar and Pump Van IfT Van Aero Van Mast Aero Van Bow Tower Fig. 1 Cruise track of R/V Ronald H. Brown during the ACE- Asia campaign. The day of year is presented at the corresponding locations of the ship. SIO Van Fig. 2 Locations of vans and a tower on R/V Ronald H. Brown. Vol. No.

3 California Riverside San Diego Aerosol Time-of-Flight Mass Spectrometry ATOFMS EDX Energy Dispersive X-ray spectrometer ATOFMS IfTTandem Differential Mobility AnalyzerTDMA TDMA Princeton FT-IRFourier Transform Infrared Spectroscopy Micro-Orifice Uniform Deposit Impactor Fig. IfT van GC- FIDGas Chromatography-Frame Ionization Detector GC-MSGas Chromatography-Mass Spectrometry California Princeton Rutgers NOAA RHB Fig. 3 RHB -,, aorganic Carbon Concentration g m btotal Dicarboxylic Acids Concentrationng m ctotal Fatty Acids Concentrationng m dlevoglucosan Concentrationng m Fig. 3 Spatial distribution of organic carbon, total dicarboxylic acids, total fatty acids, and levoglucosan in aerosols over the western North Pacific, the East China Sea, and the Sea of Japan.

4 Fig. Fig. OM OC RHB OC.. % OM/OC. OM.. % OM/OC. % DCA -COOH DCA Fig. Fig. 4 C DCAC DCA C DCAC DCA [C n DCA]/[C DCA]n,, DCA Fig. Fig. kc n DCA/kC DCA.. C -C DCA OH Kwok and Atkinson kc n DCA/kC DCA C -C DCA Relative Abundance C DCA/C DCA C DCA/C DCA C DCA/C DCA k k n n n n Oxalic Acid Concentrationng m Fig. 4 Relative abundances of C -C dicarboxylic acids to oxalic acid for all aerosol samples collected during the cruisemochida et al., Vol. No.

5 Fig. 5a LFA HFA LFA HFA LFA/HFA Fig. b LFA/HFA. LFA MSAFig. c LFA LFA nss-ca Fig. d Fig. e % ACE-Asia RHB Fatty Acidsng m MSAng m Levoglucosanng m afatty Acids b cmsa LFAs HFAs dnss-ca Levoglucosan [LFAs]/[HFAs] Day of YearUTC Fig. 5 Temporal variation ofalfas and HFAs,b [LFA]/[HFA] ratios,cmsa,dnss-ca, ande levoglucosan in aerosols during the cruisemochida et al., [LFAs]/[HFAs] nss-ca g m

6 RHB NOAA ACE-Asia References Mochida, M., Kawamura, K., Umemoto, N., Kobayashi, M., Matsunaga, S., Lim, H.-J., Turpin, B. J., Bates, T. S. and Simoneit, B. R. T.: Spatial distributions of oxygenated organic compounds dicarboxylic acids, fatty acids, and levoglucosanin marine aerosols over the western Pacific and off the coast of East Asia: Continental outflow of organic aerosols during the ACE-Asia campaign, J. Geophys. Res., 108,, doi:./ JD Mochida, M., Umemoto, N., Kawamura, K. and Uematsu, M.: Bimodal size distribution of C -C dicarboxylic acids in the marine aerosols, Geophys. Res. Lett., 30,, doi:./ GL Huebert, B. J., Bates, T., Russell, P. B., Shi, G., Kim, Y. J., Kawamura, K., Carmichael, G. and Nakajima, T.: An overview of ACE-Asia: Strategies for quantifying the relationships between Asian aerosols and their climatic impacts, J. Geophys. Res., 108,, doi:./jd Lim, H.-J., Turpin, B. J., Russell, L. M. and Bates, T. S.: Organic and elemental carbon measurements during ACE-Asia suggest a longer atmospheric lifetime for elemental carbon, Environ. Sci. Technol., 37, - Kawamura, K. and Kaplan, I. R.: Motor exhaust emissions as a primary source for dicarboxylic acids in Los Angeles ambient air, ibid., 21, - Rogge, W. F., Hildemann, L. M., Mazurek, M. A., Cass, G. R. and Simoneit, B. R. T.: Sources of fine organic aerosol:. Pine, oak, and synthetic log combustion in residential fireplaces, ibid., 32, - Satsumabayashi, H., Kurita, H., Yokouchi, Y. and Ueda, H.: Photochemical formation of particulate dicarboxylic acids under long-range transport in central Japan, Atmos. Environ., 24, - Warneck, P.: In-cloud chemistry opens pathway to the formation of oxalic acid in the marine atmosphere, ibid., 37, - Rogge, W. F., Hildemann, L. M., Mazurek, M. A., Cass, G. R. and Simoneit, B. R. T.: Sources of fine organic aerosol:. Particulate abrasion products from leaf surfaces of urban plants, Environ. Sci. Technol., 27, - Matsumoto, G. and Hanya, T.: Organic constituents in atmospheric fallout in the Tokyo area, Atmos. Environ., 14, - Mochida, M., Kitamori, Y., Kawamura, K., Nojiri, Y. and Suzuki, K.: Fatty acids in the marine atmosphere: Factors governing their concentrations and evaluation of organic films on sea-salt particles, J. Geophys. Res., 107,, doi:./ JD Rogge, W. F., Hildemann, L. M., Mazurek, M. A., Cass, G. R. and Simoneit, B. R. T.: Sources of fine organic aerosol:. Charbroilers and meat cooking operations, Environ. Sci. Technol., 25, - Rogge, W. F., Hildemann, L. M., Mazurek, M. A., Cass, G. R. and Simoneit, B. R. T.: Sources of fine organic aerosol:. Noncatalyst and catalyst-equipped automobiles and heavy-duty diesel trucks, ibid., 27, - Turpin, B. J. and Lim, H.-J.: Species contributions to PM. mass concentrations: Revisiting common assumptions for estimating organic mass, Aerosol Sci. Technol., 35, - Cruz, C. N. and Pandis, S. N.: A study of the ability of pure secondary organic aerosol to act as cloud condensation nuclei, Atmos. Environ., 31, - Mochida, M., Kawabata, A., Kawamura, K., Hatsushika, H. and Yamazaki, K.: Seasonal variation and origins of dicarboxylic acids in the marine atmosphere over the western North Pacific, J. Geophys. Res., 108,, doi:./jd Zuo, Y. and Hoigné, J.: Formation of hydrogen peroxide and depletion of oxalic acid in atmospheric water by photolysis of IronIII-oxalato complexes, Environ. Sci. Technol., 26, - Kwok, E. S. C. and Atkinson, R.: Estimation of hydroxyl radical reaction rate constants for gas-phase organic compounds using a structure-reactivity relationship: An update, Atmos. Environ., 29, - Blanchard, D. C.: Sea-to-air transport of surface active material, Science, 146, - Ellison, G. B., Tuck, A. F. and Vaida, V.: Atmospheric processing of organic aerosols, J. Geophys. Res., 104, - Peltzer, E. T., Alford, J. B. and Gagosian, R. B.: Methodology for sampling and analysis of lipids in aerosols from the remote marine atmosphere, Tech. Rep. -, Woods Hole Oceanogr. Inst., Woods Hole, Mass. Simoneit, B. R. T. and Mazurek, M. A.: Organic matter of the troposphere: II. Natural background of biogenic lipid matter in aerosols over the rural western United States, Atmos. Environ, 16, - Matsumoto, K., Kawamura, K., Uchida, M., Shibata, Y. and Yoneda, Y.: Compound specific radiocarbon and d C measurements of fatty acids in a continental aerosol sample, Geophys. Res. Lett., 28, - Schauer, J. J., Kleeman, M. J., Cass, G. R. and Simoneit, B. R. T.: Measurement of emissions from air pollution sources:. C - C organic compounds from fireplace combustion of wood, Environ. Sci. Technol., 35, - Gao, S., Hegg, D. A., Hobbs, P. V., Kirchstetter, T. W., Magi, B. I. and Sadilek, M.: Water-soluble organic components in aerosols associated with savanna fires in southern Africa: Identification, evolution, and distribution, J. Geophys. Res., 108,, doi:./jd Vol. No.

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