References

ACP

Atmospheric Chemistry and Physics

ACP

Atmos. Chem. Phys.

1680-7324

Copernicus Publications

Göttingen, Germany

10.5194/acp-12-10911-2012

The effect of model spatial resolution on Secondary Organic Aerosol predictions: a case study at Whistler, BC, Canada

Wainwright

C. D.

¹ Pierce

J. R.

¹ Liggio

² Strawbridge

K. B.

² Macdonald

A. M.

² Leaitch

R. W.

Department of Physics and Atmospheric Science, Dalhousie University, Halifax, NS, Canada

Environment Canada, Toronto, Ontario, Canada

20 11 2012

12 22 10911 10923

2012

This work is licensed under the Creative Commons Attribution 3.0 Unported License. To view a copy of this licence, visit https://creativecommons.org/licenses/by/3.0/

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A large fraction of submicron aerosol mass throughout the continental boundary layer consists of secondary organic aerosol (SOA) mass. As such, the ability of chemical transport models to accurately predict continental boundary layer aerosol greatly depends on their ability to predict SOA. Although there has been much recent effort to better describe SOA formation mechanisms in models, little attention has been paid to the effects of model spatial resolution on SOA predictions. The Whistler Aerosol and Cloud Study (WACS 2010), held between 22 June and 28 July 2010 and conducted at Whistler, BC, Canada provides a unique data set for testing simulated SOA predictions. The study consisted of intensive measurements of atmospheric trace gases and particles at several locations strongly influenced by biogenic sources in the region. We test the ability of the global chemical transport model GEOS-Chem to predict the aerosol concentrations during this event and throughout the campaign. Simulations were performed using three different resolutions of the model: 4° × 5° , 2° × 2.5° and 0.5° × 0.667°. Predictions of organic aerosol concentrations at Whistler were greatly dependent on the resolution; the 4° × 5° version of the model significantly under predicts organic aerosol, while the 2° × 2.5° and 0.5° × 0.667° versions are much more closely correlated with measurements. In addition, we performed a comparison between the 3 versions of the model across North America. Comparison simulations were run for both a summer case (July) and Winter case (January). For the summer case, 0.5° × 0.667° simulations predicted on average 19% more SOA than 2° × 2.5° and 32% more than 4° × 5° . For the winter case, the 0.5° × 0.667° simulations predicted 8% more SOA than the 2° × 2.5° and 23% more than the 4° × 5°. This increase in SOA with resolution is largely due to sub-grid variability of organic aerosol (OA) that leads to an increase in the partitioning of secondary organic matter to the aerosol phase at higher resolutions. SOA concentrations were further increased because the shift of secondary organic gases to SOA at higher resolutions increased the lifetime of secondary organic matter (secondary organic gases have a shorter deposition lifetime than SOA in the model). SOA precursor emissions also have smaller, but non-negligible, changes with resolution due to non-linear inputs to the MEGAN biogenic emissions scheme. These results suggest that a portion of the traditional under-prediction of SOA by global models may be due to the effects of coarse grid resolution.

References 1

Albrecht, B.: Aerosols, cloud microphysics, and fractional cloudiness, Science, 245, 1227–1230, 1989.

Barkley, M. P., Palmer, P., Ganzeveld, L., Arneth, A., Hagberg, D., Karl, T., Guenther, A., Paulot, F., Wennber, P. O., Mao, J., Kurosu, T. P., Chance, K., Muller, J-F., De Smedt, I., Roozendael, M. V., Chen, D., Wang, Y. and Yantosca, R. M.: Can a "state of the art" chemistry transport model simulate Amazonian tropospheric chemistry?, J. Geophys. Res., {116}, D16302, <a href="http://dx.doi.org/10.1029/2011JD015893">https://doi.org/10.1029/2011JD015893</a>, 2011

Brock, C. A., Murphy D. M., Bahreini R., and Middlebrook A. M.: Formation and growth of organic aerosols downwind of the Deepwater Horizon oil spill, Geophys. Res. Let., 38, L17805, <a href="http://dx.doi.org/10.1029/2011GL048541">https://doi.org/10.1029/2011GL048541</a>, 2011.

Cappa, C. D. and Jimenez, J. L.: Quantitative estimates of the volatility of ambient organic aerosol, Atmos. Chem. Phys., 10, 5409–5424, <a href="http://dx.doi.org/10.5194/acp-10-5409-2010">https://doi.org/10.5194/acp-10-5409-2010</a>, 2010.

Carlton, A.G., Bhave, P. V., Napelenok, S., Edney, E. O., Sarwar, G., Pinder, R. W., Pouliot, G., and Houyoux, M.: Treatment of Secondary Organic Aerosol in CMAQv4.7, Environ. Sci. Technol, 22, 8553–8560, <a href="http://dx.doi.org/10.1021/es100636q">https://doi.org/10.1021/es100636q</a>, 2010.

Chung, S. H. and Seinfeld, J. H.: Global distribution and climate forcing of carbonaceous aerosols, Geophys. Res. Lett., 107, 4407, <a href="http://dx.doi.org/10.1029/2001JD001397">https://doi.org/10.1029/2001JD001397</a>, 2002.

Ervens, B., Carlton, A. G., Turpin, B. J., Altieri, K. E., Kreidenweis, S. M., and Feingold, G.: Secondary organic aerosol yields from cloud-processing of isoprene oxidation products, Geophys. Res. Lett., 35, L02816, <a href="http://dx.doi.org/10.1029/2007GL031828">https://doi.org/10.1029/2007GL031828</a>, 2008.

Goldstein, A. and Galbally, I.: Known and unexplored organic constituents in the earth's atmosphere, Environ. Sci. Technol., 41, 1514–1521, 2007.

Guenther, A., Karl, T., Harley, P., Wiedinmyer, C., Palmer, P. I., and Geron, C.: Estimates of global terrestrial isoprene emissions using MEGAN (Model of Emissions of Gases and Aerosols from Nature), Atmos. Chem. Phys., 6, 3181–3210, <a href="http://dx.doi.org/10.5194/acp-6-3181-2006">https://doi.org/10.5194/acp-6-3181-2006</a>, 2006.

Hand, J. L., Schichtel, B. A., Pitchford, M., Malm, W. C., and Frank, N. H.: Seasonal composition of remote and urban fine particulate matter in the United States, {J. Geophys. Res.}, {117}, D05209, <a href="http://dx.doi.org/10.1029/2011JD017122">https://doi.org/10.1029/2011JD017122</a>, 2012.

Heald, C.L., Jacob, D. J., Park, R. J., Russell, L. M., Huebert, B. J., Seinfeld, J. H., Liao, H., and Weber, R. J.: A large organic aerosol source in the free troposphere missing from current models, Geophys. Res. Lett., 32, L18809, <a href="http://dx.doi.org/10.1029/2005GL023831">https://doi.org/10.1029/2005GL023831</a>, 2005.

Henze, D. K. and Seinfeld, J. H.: Global secondary organic aerosol from isoprene oxidation, Geophys. Res. Lett{.}, 33, L09812, <a href="http://dx.doi.org/10.1029/2006GL025976">https://doi.org/10.1029/2006GL025976</a>, 2006.

Henze, D. K., Seinfeld, J. H., Ng, N. L., Kroll, J. H., Fu, T.-M., Jacob, D. J., and Heald, C. L.: Global modeling of secondary organic aerosol formation from aromatic hydrocarbons: high- vs. low-yield pathways, Atmos. Chem. Phys., 8, 2405–2420, <a href="http://dx.doi.org/10.5194/acp-8-2405-2008">https://doi.org/10.5194/acp-8-2405-2008</a>, 2008.

Intergovernmental Panel on Climate Change: Climate Change 2007 – The Physical Science Basis: Contribution of Working Group I to the Fourth Assessment Report of the IPCC, Cambridge University press, 2007.

Jang, M. S., Czoschke, N. M., Lee, S., and Kamens, R. M.: Heterogeneous atmospheric aerosol production by acid- catalyzed particle-phase reactions, Science, 298, 814–817, <a href="http://dx.doi.org/10.1126/science.1075798">https://doi.org/10.1126/science.1075798</a>, 2002.

Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., Prevot, A.S, Zhang, Q., Kroll, J. H., DeCarlo, P. F., Allan, J. D., Coe, H., Ng, N. L., Aiken, A. C., Docherty, K. S., Ulbrich, I. M., Grieshop, A. P., Robinson, A. L., Duplissy, J., Smith, J. D., Wilson, K. R., Lanz, V. A., Hueglin, C., Sun, Y. L., Tian, J., Laaksonen, A., Raatikainen, T., Rautiainen, J., Vaattovaara, P., Ehn, M., Kulmala, M., Tomlinson, J. M., Collins, D. R., Cubison, M. J., Dunlea, E. J., Huffman, J. A., Onasch, T. B., Alfarra, M. R., Williams, P. I., Bower, K., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Salcedo, D., Cottrell, L., Griffin, R., Takami, A., Miyoshi, T., Hatakeyama, S., Shimono, A., Sun, J. Y., Zhang, Y. M., Dzepina, K., Kimmel, J. R., Sueper, D., Jayne, J. T., Herndon, S. C., Trimborn, A. M., Williams, L. R., Wood, E. C., Middlebrook, A. M., Kolb, C. E., Baltensperger, U., and Worsnop, D. R.: Evolution of Organic Aerosols in the Atmosphere, Science, 326, 1525–1529, 2009.

Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, <a href="http://dx.doi.org/10.5194/acp-5-1053-2005">https://doi.org/10.5194/acp-5-1053-2005</a>, 2005.

Kim, Y., Sartelet, K., and Seigneur, C.: Formation of secondary aerosols over Europe: comparison of two gas-phase chemical mechanisms, Atmos. Chem. Phys., 11, 583–598, <a href="http://dx.doi.org/10.5194/acp-11-583-2011">https://doi.org/10.5194/acp-11-583-2011</a>, 2011.

Lane, T.E., Donahue, N., and Pandis, S.: Simulating secondary organic aerosol formation using the volatility basis-set approach in a chemical transport model, Atmos. Environ., 32, 7439–7451, 2008.

Leaitch, R., Macdonald, A. M., Brickell, P. C., Liggio, J., Sjostedt, S. J., Vlasenko, A., Bottenheim, J. W., Huang, L., Li, S., Liu, P. S.K., Toom-Sauntry, D., Hayden, K. A., Sharma, S., Shantz, N. C., Wiebe, A., Zhang, W., Abbatt, J., Slowik, J. G., Chang, R. Y.-W., Russell, L. M., Schwartz, R. E., Takahama, S., Jayne, J. T., and Ng, N. L.: Temperature response of the submicron organic aerosol from temperate forests, Atmos. Environ., 37, 6696–6704, 2010.

Lin, G., Penner, J. E., Sillman, S., Taraborrelli, D., and Lelieveld, J.: Global modeling of SOA formation from dicarbonyls, epoxides, organic nitrates and peroxides, Atmos. Chem. Phys., 12, 4743–4774, <a href="http://dx.doi.org/10.5194/acp-12-4743-2012">https://doi.org/10.5194/acp-12-4743-2012</a>, 2012.

Macdonald, A. M., Leaitch, W. R., Abbatt, J. P. D., Ahlm, L., Al-Basheer, W., Betram, A., Buller, J., Campuzano-Jost, P., Chan, E., Corbin, J., Cziczo, D., Elford, A., Hayden, K. A., Herckes, P., Lee, A. K. Y., Li, S.-M., Liggio, J., Liu, P. S. K., Mihele, C., Noone K., Pierce, J. R., Russell, L. M., Toom-Sauntry, D., Schroder, J., Sharma, S., Sheppard, A., Sjostedt, S. J., Slowik, J. G., Strawbridge, K., Stupple, G., Vlasenko, A., Wainwright, C., Wang, Y., Wentzell, J., Wiebe, H. A., and Wong, J. P. S.: Overview of the 2010 Whistler Aerosol and Cloud Study, in preparation, 2012.

Odum, J. R., Jungkaamp, T. P. W., Griffin, R. J., Flagan, R. C., and Seinfeld, J. H.: The Atmospheric Aerosol-Forming Potential of Whole Gasoline Vapor, Science, 276, 5309, 96–99, https://doi.org/ 10.1126/science.276.5309.96, 1997.

Pankow, J. F.: An absorption model of gas/particle partitioning of organic compounds in the atmosphere, Atmos. Environ., 28A, 185–188, 1994.

Petters, M. D. and Kreidenweis, S. M.: A single parameter representation of hygroscopic growth and cloud condensation nucleus activity, Atmos. Chem. Phys., 7, 1961–1971, https://doi.org/10.5194/acp-7-1961-2007, 2007.

Pierce, J. R. and Adams, P. J.: Uncertainty in global CCN concentrations from uncertain aerosol nucleation and primary emission rates, Atmos. Chem. Phys., 9, 1339–1356, <a href="http://dx.doi.org/10.5194/acp-9-1339-2009">https://doi.org/10.5194/acp-9-1339-2009</a>, 2009.

Pierce, J. R., Riipinen, I., Kulmala, M., Ehn, M., Petäjä, T., Junninen, H., Worsnop, D. R., and Donahue, N. M.: Quantification of the volatility of secondary organic compounds in ultrafine particles during nucleation events, Atmos. Chem. Phys., 11, 9019–9036, <a href="http://dx.doi.org/10.5194/acp-11-9019-2011">https://doi.org/10.5194/acp-11-9019-2011</a>, 2011.

Pierce, J. R., Leaitch, W. R., Liggio, J., Westervelt, D. M., Wainwright, C. D., Abbatt, J. P. D., Ahlm, L., Al-Basheer, W., Cziczo, D. J., Hayden, K. L., Lee, A. K. Y., Li, S.-M., Russell, L. M., Sjostedt, S. J., Strawbridge, K. B., Travis, M., Vlasenko, A., Wentzell, J. J. B., Wiebe, H. A., Wong, J. P. S., and Macdonald, A. M.: Nucleation and condensational growth to CCN sizes during a sustained pristine biogenic SOA event in a forested mountain valley, Atmos. Chem. Phys., 12, 3147–3163, <a href="http://dx.doi.org/10.5194/acp-12-3147-2012">https://doi.org/10.5194/acp-12-3147-2012</a>, 2012.

Robinson, A. L., Donahue, N. M., Shrivastava, M. K., Weitkamp, E. A., Sage, A. M., Grieshop, A. P., Lane, T. E., Pierce, J. R., and Pandis, S. N: Rethinking organic aerosols: Semivolatile emissions and photochemical aging, Science, 315, 1259–1262, 2007.

Riipinen, I., Pierce, J. R., Yli-Juuti, T., Nieminen, T., Häkkinen, S., Ehn, M., Junninen, H., Lehtipalo, K., Petäjä, T., Slowik, J., Chang, R., Shantz, N. C., Abbatt, J., Leaitch, W. R., Kerminen, V.-M., Worsnop, D. R., Pandis, S. N., Donahue, N. M., and Kulmala, M.: Organic condensation: a vital link connecting aerosol formation to cloud condensation nuclei (CCN) concentrations, Atmos. Chem. Phys., 11, 3865–3878, <a href="http://dx.doi.org/10.5194/acp-11-3865-2011">https://doi.org/10.5194/acp-11-3865-2011</a>, 2011.

Shilling, J. E., Chen, Q., King, S. M., Rosenoern, T., Kroll, J. H., Worsnop, D. R., McKinney, K. A., and Martin, S. T.: Particle mass yield in secondary organic aerosol formed by the dark ozonolysis of α-pinene, Atmos. Chem. Phys., 8, 2073–2088, https://doi.org/10.5194/acp-8-2073-2008, 2008.

Shiraiwa, M., Ammann, M., Koop, T., and Pöschl, U.: Gas uptake and chemical aging of semisolid organic aerosol particles, P. Natl. Acad. Sci., 108, 11003–11008, 2011.

Spracklen, D. V., Jimenez, J. L., Carslaw, K. S., Worsnop, D. R., Evans, M. J., Mann, G. W., Zhang, Q., Canagaratna, M. R., Allan, J., Coe, H., McFiggans, G., Rap, A., and Forster, P.: Aerosol mass spectrometer constraint on the global secondary organic aerosol budget, Atmos. Chem. Phys., 11, 12109–12136, <a href="http://dx.doi.org/10.5194/acp-11-12109-2011">https://doi.org/10.5194/acp-11-12109-2011</a>, 2011.

Stroud, C. A., Makar, P. A., Moran, M. D., Gong, W., Gong, S., Zhang, J., Hayden, K., Mihele, C., Brook, J. R., Abbatt, J. P. D., and Slowik, J. G.: Impact of model grid spacing on regional- and urban-scale air quality predictions of organic aerosol, Atmos. Chem. Phys., 11, 3107–3118, <a href="http://dx.doi.org/10.5194/acp-11-3107-2011">https://doi.org/10.5194/acp-11-3107-2011</a>, 2011.

Twomey, S.: Pollution and the Planetary Albedo, Atmos. Environ., 8, 1251–6, <a href="http://dx.doi.org/10.1016/0004-6981(74)90004-3">https://doi.org/10.1016/0004-6981(74)90004-3</a>, 1974.

Vaden T. D., Imre, D. G., Beranek, J., Shrivastava, M. K. B., and Zelenyuk, A.: Evaporation Kinetics and Phase of Laboratory and Ambient Secondary Organic Aerosol, P. Natl. Acad. Sci. USA, 108, 2190–2195, <a href="http://dx.doi.org/10.1073/pnas.1013391108">https://doi.org/10.1073/pnas.1013391108</a>, 2010.

van Donkelaar, A., Martin, R. V., Leaitch, W. R., Macdonald, A. M., Walker, T. W., Streets, D. G., Zhang, Q., Dunlea, E. J., Jimenez, J. L., Dibb, J. E., Huey, L. G., Weber, R., and Andreae, M. O.: Analysis of aircraft and satellite measurements from the Intercontinental Chemical Transport Experiment (INTEX-B) to quantify long-range transport of East Asian sulfur to Canada, Atmos. Chem. Phys., 8, 2999–3014, <a href="http://dx.doi.org/10.5194/acp-8-2999-2008">https://doi.org/10.5194/acp-8-2999-2008</a>, 2008.

van Donkelaar, A.: Global estimates of ambient fine particulate matter concentrations from satellite-based aerosol optical depth: Development and application, Environ. Health. Perspec., 118, 847–855, <a href="http://dx.doi.org/10.1289/ehp.0901623">https://doi.org/10.1289/ehp.0901623</a>, 2010.

Volkamer, R., Jimenez, J. L., Dzepina, K., Salcedo, D., SanMartini, F. M., Molina, L. T., Worsnop, D. R., and Molina, M. J.: Secondary Organic Aerosol formation from Anthropogenic Air Pollution: Rapid and higher than expected, Geophys. Res. Lett., 33, L17811, <a href="http://dx.doi.org/10.1029/2006GL026899">https://doi.org/10.1029/2006GL026899</a>, 2006.

Weigum, N. M., Stier, P., Schwarz, J. P., Fahey, D. W., and Spackman, J. R.: Scales of variability of black carbon plumes over the Pacific Ocean, Geophys. Res. Lett., 39, L15804, <a href="http://dx.doi.org/10.1029/2012GL052127">https://doi.org/10.1029/2012GL052127</a>, 2012.