References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-11-6895-2011

Explicit modelling of SOA formation from α-pinene photooxidation: sensitivity to vapour pressure estimation

Valorso

¹ Aumont

¹ Camredon

¹ Raventos-Duran

¹ Mouchel-Vallon

¹ Ng

N. L.

² Seinfeld

J. H.

³ Lee-Taylor

⁴ Madronich

⁴

LISA, UMR CNRS/INSU 7583, Université Paris Est Créteil et Université Paris Diderot, Institut Pierre Simon Laplace, 94010 Créteil Cedex, France

Aerodyne Research, Inc. Billerica, MA 01821, USA

California Institute of Technology, Pasadena, CA 91125, USA

Atmospheric Chemistry Division, NCAR, Boulder, CO, USA

18 07 2011

11 14 6895 6910

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

This article is available from http://www.atmos-chem-phys.net/11/6895/2011/acp-11-6895-2011.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/11/6895/2011/acp-11-6895-2011.pdf

The sensitivity of the formation of secondary organic aerosol (SOA) to the estimated vapour pressures of the condensable oxidation products is explored. A highly detailed reaction scheme was generated for α-pinene photooxidation using the Generator for Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A). Vapour pressures (Pvap) were estimated with three commonly used structure activity relationships. The values of Pvap were compared for the set of secondary species generated by GECKO-A to describe α-pinene oxidation. Discrepancies in the predicted vapour pressures were found to increase with the number of functional groups borne by the species. For semi-volatile organic compounds (i.e. organic species of interest for SOA formation), differences in the predicted Pvap range between a factor of 5 to 200 on average. The simulated SOA concentrations were compared to SOA observations in the Caltech chamber during three experiments performed under a range of NOx conditions. While the model captures the qualitative features of SOA formation for the chamber experiments, SOA concentrations are systematically overestimated. For the conditions simulated, the modelled SOA speciation appears to be rather insensitive to the Pvap estimation method.

References 1

Aiken, A. C., DeCarlo, P. F., Kroll, J. H., Worsnop, D. R., Huffman, J. A., Docherty, K. S., Ulbrich, I. M., Mohr, C., Kimmel, J. R., Sueper, D., Sun, Y., Zhang, Q., Trimborn, A., Northway, M., Ziemann, P. J., Canagaratna, M. R., Onasch, T. B., Alfarra, M. R., Prevot, A. S. H., Dommen, J., Duplissy, J., Metzger, A., Baltensperger, U., and Jimenez, J. L.: O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry, Environ. Sci. Technol., 42, 4478–4485, 2008.

Atkinson, R.: Atmospheric chemistry of VOCs and NOx, Atmos. Environ., 34, 2063–2101, 2000.

Aumont, B., Szopa, S., and Madronich, S.: Modelling the evolution of organic carbon during its gas-phase tropospheric oxidation: development of an explicit model based on a self generating approach, Atmos. Chem. Phys., 5, 2497–2517, http://dx.doi.org/10.5194/acp-5-2497-2005doi:10.5194/acp-5-2497-2005, 2005.

Barley, M. H. and McFiggans, G.: The critical assessment of vapour pressure estimation methods for use in modelling the formation of atmospheric organic aerosol, Atmos. Chem. Phys., 10, 749–767, http://dx.doi.org/10.5194/acp-10-749-2010doi:10.5194/acp-10-749-2010, 2010.

Booth, A. M., Barley, M. H., Topping, D. O., McFiggans, G., Garforth, A., and Percival, C. J.: Solid state and sub-cooled liquid vapour pressures of substituted dicarboxylic acids using Knudsen Effusion Mass Spectrometry (KEMS) and Differential Scanning Calorimetry, Atmos. Chem. Phys., 10, 4879–4892, http://dx.doi.org/10.5194/acp-10-4879-2010doi:10.5194/acp-10-4879-2010, 2010.

Booth, A. M., Montague, W. J., Barley, M. H., Topping, D. O., McFiggans, G., Garforth, A., and Percival, C. J.: Solid state and sub-cooled liquid vapour pressures of cyclic aliphatic dicarboxylic acids, Atmos. Chem. Phys., 11, 655–665, http://dx.doi.org/10.5194/acp-11-655-2011doi:10.5194/acp-11-655-2011, 2011.

Camredon, M. and Aumont, B.: Assessment of vapor pressure estimation methods for secondary organic aerosol modeling, Atmos. Environ., 40, 2105–2116, http://dx.doi.org/10.1016/j.atmosenv.2005.11.051doi:10.1016/j.atmosenv.2005.11.051, 2006.

Camredon, M., Aumont, B., Lee-Taylor, J., and Madronich, S.: The SOA/VOC/NOx system: an explicit model of secondary organic aerosol formation, Atmos. Chem. Phys., 7, 5599–5610, http://dx.doi.org/10.5194/acp-7-5599-2007doi:10.5194/acp-7-5599-2007, 2007.

Camredon, M., Hamilton, J. F., Alam, M. S., Wyche, K. P., Carr, T., White, I. R., Monks, P. S., Rickard, A. R., and Bloss, W. J.: Distribution of gaseous and particulate organic composition during dark ?-pinene ozonolysis, Atmos. Chem. Phys., 10, 2893–2917, http://dx.doi.org/10.5194/acp-10-2893-2010doi:10.5194/acp-10-2893-2010, 2010.

Capouet, M. and Müller, J.-F.: A group contribution method for estimating the vapour pressures of α-pinene oxidation products, Atmos. Chem. Phys., 6, 1455–1467, http://dx.doi.org/10.5194/acp-6-1455-2006doi:10.5194/acp-6-1455-2006, 2006.

Capouet, M., Muller, J. F., Ceulemans, K., Compernolle, S., Vereecken, L., and Peeters, J.: Modeling aerosol formation in alpha-pinene photo-oxidation experiments, J. Geophys. Res.-Atmos., 113(22), D02308 http://dx.doi.org/10.1029/2007jd008995doi:10.1029/2007jd008995, 2008.

Cappa, C. D. and Wilson, K. R.: Evolution of organic aerosol mass spectra upon heating: implications for OA phase and partitioning behavior, Atmos. Chem. Phys., 11, 1895–1911, http://dx.doi.org/10.5194/acp-11-1895-2011doi:10.5194/acp-11-1895-2011, 2011.

Chhabra, P. S., Ng, N. L., Canagaratna, M. R., Corrigan, A. L., Russell, L. M., Worsnop, D. R., Flagan, R. C., and Seinfeld, J. H.: Elemental composition and oxidation of chamber organic aerosol, Atmos. Chem. Phys. Discuss., 11, 10305–10342, http://dx.doi.org/10.5194/acpd-11-10305-2011doi:10.5194/acpd-11-10305-2011, 2011.

Clegg, S. L., Kleeman, M. J., Griffin, R. J., and Seinfeld, J. H.: Effects of uncertainties in the thermodynamic properties of aerosol components in an air quality model – Part 2: Predictions of the vapour pressures of organic compounds, Atmos. Chem. Phys., 8, 1087–1103, http://dx.doi.org/10.5194/acp-8-1087-2008doi:10.5194/acp-8-1087-2008, 2008.

Compernolle, S., Ceulemans, K., and Müller, J.-F.: Technical Note: Vapor pressure estimation methods applied to secondary organic aerosol constituents from α-pinene oxidation: an intercomparison study, Atmos. Chem. Phys., 10, 6271–6282, http://dx.doi.org/10.5194/acp-10-6271-2010doi:10.5194/acp-10-6271-2010, 2010.

Donahue, N. M., Robinson, A. L., and Pandis, S. N.: Atmospheric organic particulate matter: From smoke to secondary organic aerosol, Atmos. Environ., 43, 94–106, http://dx.doi.org/10.1016/j.atmosenv.2008.09.055doi:10.1016/j.atmosenv.2008.09.055, 2009.

Fuzzi, S., Andreae, M. O., Huebert, B. J., Kulmala, M., Bond, T. C., Boy, M., Doherty, S. J., Guenther, A., Kanakidou, M., Kawamura, K., Kerminen, V.-M., Lohmann, U., Russell, L. M., and Pöschl, U.: Critical assessment of the current state of scientific knowledge, terminology, and research needs concerning the role of organic aerosols in the atmosphere, climate, and global change, Atmos. Chem. Phys., 6, 2017–2038, http://dx.doi.org/10.5194/acp-6-2017-2006doi:10.5194/acp-6-2017-2006, 2006.

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

Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, Th. F., Monod, A., Prévôt, A. S. H., Seinfeld, J. H., Surratt, J. D., Szmigielski, R., and Wildt, J.: The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, http://dx.doi.org/10.5194/acp-9-5155-2009doi:10.5194/acp-9-5155-2009, 2009.

Heaton, K. J., Dreyfus, M. A., Wang, S., and Johnston, M. V.: Oligomers in the early stage of biogenic secondary organic aerosol formation and growth, Environ. Sci. Technol., 41, 6129–6136, http://dx.doi.org/10.1021/es070314ndoi:10.1021/es070314n, 2007.

Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., Prevot, A. S. H., 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, http://dx.doi.org/10.1126/science.1180353doi:10.1126/science.1180353, 2009.

Joback, K. G. and Reid, R. C.: Estimation of Pure-Component Properties from Group-Contributions, Chem. Eng. Commun., 57, 233–243, 1987.

Kalberer, M., Paulsen, D., Sax, M., Steinbacher, M., Dommen, J., Prevot, A. S. H., Fisseha, R., Weingartner, E., Frankevich, V., Zenobi, R., and Baltensperger, U.: Identification of polymers as major components of atmospheric organic aerosols, Science, 303, 1659–1662, 2004.

Kroll, J. H. and Seinfeld, J. H.: Chemistry of secondary organic aerosol: Formation and evolution of low-volatility organics in the atmosphere, Atmos. Environ., 42, 3593–3624, http://dx.doi.org/10.1016/j.atmosenv.2008.01.003doi:10.1016/j.atmosenv.2008.01.003, 2008.

Kroll, J. H., Smith, J. D., Che, D. L., Kessler, S. H., Worsnop, D. R., and Wilson, K. R.: Measurement of fragmentation and functionalization pathways in the heterogeneous oxidation of oxidized organic aerosol, Phys. Chem. Chem. Phys., 11, 8005–8014, http://dx.doi.org/10.1039/b905289edoi:10.1039/b905289e, 2009.

Kroll, J. H., Donahue, N., Jimenez, J. L., Kessler, S. H., Canagaratna, M. R., Wilson, E. R., Altieri, K. E., R., M. L., Wozniak, A. S., Bluhm, H., Mysak, E. R., Smith, J. D., Kolb, C. E., and Worsnop, D. R.: Carbon oxidation state as a metric for describing the chemistry of atmospheric organic aerosol, Nature Chemistry, 3, 133–139, 2011.

Loza, C. L., Chan, A. W. H., Galloway, M. M., Keutsch, F. N., Flagan, R. C., and Seinfeld, J. H.: Characterization of Vapor Wall Loss in Laboratory Chambers, Environ. Sci. Technol., 44, 5074–5078, http://dx.doi.org/10.1021/es100727vdoi:10.1021/es100727v, 2010.

Matsunaga, A. and Ziemann, P.: Gas-wall partitioning of organic compounds in a teflon film chamber and potential effects on reaction product and aerosol yield measurements, Aerosol Sci. Technol., 44, 881–892, 2010.

Molina, M. J., Ivanov, A. V., Trakhtenberg, S., and Molina, L. T.: Atmospheric evolution of organic aerosol, Geophys. Res. Lett., 31(5), L22104 http://dx.doi.org/10.1029/2004gl020910doi:10.1029/2004gl020910, 2004.

Moller, B., Rarey, J., and Ramjugernath, D.: Estimation of the vapour pressure of non-electrolyte organic compounds via group contributions and group interactions, J. Mol. Liq., 143, 52–63, http://dx.doi.org/10.1016/j.molliq.2008.04.020doi:10.1016/j.molliq.2008.04.020, 2008.

Myrdal, P. B. and Yalkowsky, S. H.: Estimating pure component vapor pressures of complex organic molecules, Ind. Eng. Chem. Res., 36, 2494–2499, 1997.

Nannoolal, Y., Rarey, J., Ramjugernath, D., and Cordes, W.: Estimation of pure component properties: Part 1. Estimation of the normal boiling point of non-electrolyte organic compounds via group contributions and group interactions, Fluid Phase Equilibria, 226, 45–63, 2004.

Nannoolal, Y., Rarey, J., and Ramjugernath, D.: Estimation of pure component properties: Part 3. Estimation of the vapor pressure of non-electrolyte organic compounds via group contributions and group interactions, Fluid Phase Equilibria, 269, 117–133, 2008.

Ng, N. L., Chhabra, P. S., Chan, A. W. H., Surratt, J. D., Kroll, J. H., Kwan, A. J., McCabe, D. C., Wennberg, P. O., Sorooshian, A., Murphy, S. M., Dalleska, N. F., Flagan, R. C., and Seinfeld, J. H.: Effect of NOx level on secondary organic aerosol (SOA) formation from the photooxidation of terpenes, Atmos. Chem. Phys., 7, 5159–5174, http://dx.doi.org/10.5194/acp-7-5159-2007doi:10.5194/acp-7-5159-2007, 2007.

Ng, N. L., Canagaratna, M. R., Zhang, Q., Jimenez, J. L., Tian, J., Ulbrich, I. M., Kroll, J. H., Docherty, K. S., Chhabra, P. S., Bahreini, R., Murphy, S. M., Seinfeld, J. H., Hildebrandt, L., Donahue, N. M., DeCarlo, P. F., Lanz, V. A., Prévôt, A. S. H., Dinar, E., Rudich, Y., and Worsnop, D. R.: Organic aerosol components observed in Northern Hemispheric datasets from Aerosol Mass Spectrometry, Atmos. Chem. Phys., 10, 4625–4641, http://dx.doi.org/10.5194/acp-10-4625-2010doi:10.5194/acp-10-4625-2010, 2010.

Ng, N. L., Canagaratna, M. R., Jimenez, J. L., Chhabra, P. S., Seinfeld, J. H., and Worsnop, D. R.: Changes in organic aerosol composition with aging inferred from aerosol mass spectra, Atmos. Chem. Phys., 11, 6465–6474, http://dx.doi.org/10.5194/acp-11-6465-2011doi:10.5194/acp-11-6465-2011, 2011.

Noziere, B., Barnes, I., and Becker, K. H.: Product study and mechanisms of the reactions of alpha-pinene and of pinonaldehyde with OH radicals, J. Geophys. Res.-Atmos., 104, 23645–23656, 1999.

Pankow, J. F.: An Absorption-Model of the Gas Aerosol Partitioning Involved in the Formation of Secondary Organic Aerosol, Atmos. Environ., 28, 189–193, 1994.

Pankow, J. F. and Asher, W. E.: SIMPOL.1: a simple group contribution method for predicting vapor pressures and enthalpies of vaporization of multifunctional organic compounds, Atmos. Chem. Phys., 8, 2773–2796, http://dx.doi.org/10.5194/acp-8-2773-2008doi:10.5194/acp-8-2773-2008, 2008.

Peeters, J., Vereecken, L., and Fantechi, G.: The detailed mechanism of the OH-initiated atmospheric oxidation of alpha-pinene: a theoretical study, Phys. Chem. Chem. Phys., 3, 5489–5504, 2001.

Pinho, P. G., Pio, C. A., Carter, W. P. L., and Jenkin, M. E.: Evaluation of alpha- and beta-pinene degradation in the detailed tropospheric chemistry mechanism, MCM v3.1, using environmental chamber data, J. Atmos. Chem., 57, 171–202, http://dx.doi.org/10.1007/s10874-007-9071-0doi:10.1007/s10874-007-9071-0, 2007.

Reinnig, M. C., Warnke, J., and Hoffmann, T.: Identification of organic hydroperoxides and hydroperoxy acids in secondary organic aerosol formed during the ozonolysis of different monoterpenes and sesquiterpenes by on-line analysis using atmospheric pressure chemical ionization ion trap mass spectrometry, Rapid Commun. Mass Spectrom., 23, 1735–1741, http://dx.doi.org/10.1002/rcm.4065doi:10.1002/rcm.4065, 2009.

Rollins, A. W., Smith, J. D., Wilson, K. R., and Cohen, R. C.: Real Time In Situ Detection of Organic Nitrates in Atmospheric Aerosols, Environ. Sci. Technol., 44, 5540–5545, http://dx.doi.org/10.1021/es100926xdoi:10.1021/es100926x, 2010.

Saunders, S. M., Jenkin, M. E., Derwent, R. G., and Pilling, M. J.: Protocol for the development of the Master Chemical Mechanism, MCM v3 (Part A): tropospheric degradation of non-aromatic volatile organic compounds, Atmos. Chem. Phys., 3, 161–180, http://dx.doi.org/10.5194/acp-3-161-2003doi:10.5194/acp-3-161-2003, 2003.

Vaden, T. D., Imre, D., Beranek, J., Shrivastava, M., and Zelenyuk, A.: Evaporation kinetics and phase of laboratory and ambient secondary organic aerosol, Proc. Natl. Acad. Sci. USA, 108, 2190–2195, http://dx.doi.org/10.1073/pnas.1013391108doi:10.1073/pnas.1013391108, 2011.

Verwer, J. G. and Vanloon, M.: An Evaluation of Explicit Pseudo-Steady-State Approximation Schemes for Stiff Ode Systems from Chemical-Kinetics, J. Comput. Phys., 113, 347–352, 1994.

Verwer, J. G., Blom, J. G., VanLoon, M., and Spee, E. J.: A comparison of stiff ODE solvers for atmospheric chemistry problems, Atmos. Environ., 30, 49–58, 1996.

Virtanen, A., Joutsensaari, J., Koop, T., Kannosto, J., Yli-Pirila, P., Leskinen, J., Makela, J. M., Holopainen, J. K., Poschl, U., Kulmala, M., Worsnop, D. R., and Laaksonen, A.: An amorphous solid state of biogenic secondary organic aerosol particles, Nature, 467, 824–827, 10.1038/nature09455, 2010.

Xia, A. G., Michelangeli, D. V., and Makar, P. A.: Box model studies of the secondary organic aerosol formation under different HC/NOx conditions using the subset of the Master Chemical Mechanism for alpha-pinene oxidation, J. Geophys. Res., 113, D10301, http://dx.doi.org/10.1029/2007JD008726doi:10.1029/2007JD008726, 2008.