Effects of molecular weight and temperature on liquid-liquid phase separation in particles containing organic species and inorganic salts

Atmospheric Chemistry and Physics

Volumn 15, Issue 3, 2015, Pages 1351-1365

  You, Y ^a   Bertram, A K ^a  

^a UNIVERSITY OF BRITISH COLUMBIA   (Canada)

Author keywords

[No Author keywords available]

Indexed keywords

AMMONIUM SULFATE; DIFFUSION; INORGANIC SALT; PARAMETERIZATION; PARTICLE SIZE; PARTICULATE MATTER; RELATIVE HUMIDITY;

EID: 84922573358     PISSN: 16807316     EISSN: 16807324     Source Type: Journal    
DOI: 10.5194/acp-15-1351-2015     Document Type: Article

References (115)

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., Prévôt, 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 highresolution time-of-flight aerosol mass spectrometry, Environ. Sci. Technol., 42, 4478-4485, doi:10.1021/es703009q, 2008.
2. Anttila, T., Kiendler-Scharr, A., Tillmann, R., and Mentel, T. F.: On the reactive uptake of gaseous compounds by organic-coated aqueous aerosols: Theoretical analysis and application to the heterogeneous hydrolysis of N2O5, J. Phys. Chem. A, 110, 10435-10443, doi:10.1021/jp062403c, 2006.
3. Anttila, T., Kiendler-Scharr, A., Mentel, T. F., and Tillmann, R.: Size dependent partitioning of organic material: evidence for the formation of organic coatings on aqueous aerosols, J. Atmos. Chem., 57, 215-237, doi:10.1007/s10874-007-9067-9, 2007.
4. Badger, C. L., George, I., Griffiths, P. T., Braban, C. F., Cox, R. A., and Abbatt, J. P. D.: Phase transitions and hygroscopic growth of aerosol particles containing humic acid and mixtures of humic acid and ammonium sulfate, Atmos. Chem. Phys., 6, 755-768, 2006, http://www.atmos-chem-phys.net/6/755/2006/.
5. Bertram, A. K., Martin, S. T., Hanna, S. J., Smith, M. L., Bodsworth, A., Chen, Q., Kuwata, M., Liu, A., You, Y., and Zorn, S. R.: Predicting the relative humidities of liquid-liquid phase separation, efflorescence, and deliquescence of mixed particles of ammonium sulfate, organic material, and water using the organic-to-sulfate mass ratio of the particle and the oxygen-tocarbon elemental ratio of the organic component, Atmos. Chem. Phys., 11, 10995-11006, doi:10.5194/acp-11-10995-2011, 2011.
6. Bodsworth, A., Zobrist, B., and Bertram, A. K.: Inhibition of efflorescence in mixed organic-inorganic particles at temperatures less than 250 K, Phys. Chem. Chem. Phys., 12, 12259-12266, doi:10.1039/c0cp00572j, 2010.
7. Braban, C. F. and Abbatt, J. P. D.: A study of the phase transition behavior of internally mixed ammonium sulfate-malonic acid aerosols, Atmos. Chem. Phys., 4, 1451-1459, doi:10.5194/acp-4-1451-2004, 2004.
8. Brooks, S. D., Wise, M. E., Cushing, M., and Tolbert, M. A.: Deliquescence behavior of organic/ammonium sulfate aerosol, Geophys. Res. Lett., 29, 1917, doi:10.1029/2002GL014733, 2002.
9. Brooks, S. D., Garland, R. M., Wise, M. E., Prenni, A. J., Cushing, M., Hewitt, E., and Tolbert, M. A.: Phase changes in internally mixed maleic acid/ammonium sulfate aerosols, J. Geophys. Res., 108, 4478, doi:10.1029/2002jd003204, 2003.
10. Buajarern, J., Mitchem, L., and Reid, J. P.: Characterizing multiphase Organic/Inorganic/Aqueous aerosol droplets, J. Phys. Chem. A, 111, 9054-9061, doi:10.1021/jp074366a, 2007.
11. Buzorius, G., Zelenyuk, A., Brechtel, F., and Imre, D.: Simultaneous determination of individual ambient particle size, hygroscopicity and composition, Geophys. Res. Lett., 29, 1974, doi:10.1029/2001GL014221, 2002.
12. Chan, M. N., and Chan, C. K.: Hygroscopic properties of two model humic-like substances and their mixtures with inorganics of atmospheric importance, Environ. Sci. Technol., 37, 5109-5115, doi:10.1021/es034272o, 2003.
13. Chang, E. I. and Pankow, J. F.: Prediction of activity coefficients in liquid aerosol particles containing organic compounds, dissolved inorganic salts, and water-Part 2: Consideration of phase separation effects by an X-UNIFAC model, Atmos. Environ., 40, 6422-6436, doi:10.1016/j.atmosenv.2006.04.031, 2006.
14. Chen, Q., Farmer, D. K., Schneider, J., Zorn, S. R., Heald, C. L., Karl, T. G., Guenther, A., Allan, J. D., Robinson, N., Coe, H., Kimmel, J. R., Pauliquevis, T., Borrmann, S., Pöschl, U., Andreae, M. O., Artaxo, P., Jimenez, J. L., and Martin, S. T.: Mass spectral characterization of submicron biogenic organic particles in the Amazon Basin, Geophys. Res. Lett., 36, L20806, doi:10.1029/2009GL039880, 2009.
15. Choi, M. Y. and Chan, C. K.: The effects of organic species on the hygroscopic behaviors of inorganic aerosols, Environ. Sci. Technol., 36, 2422-2428, doi:10.1021/es0113293, 2002.
16. Ciobanu, V. G., Marcolli, C., Krieger, U. K., Weers, U., and Peter, T.: Liquid-liquid phase separation in mixed organic/inorganic aerosol particles, J. Phys. Chem. A, 113, 10966-10978, doi:10.1021/jp905054d, 2009.
17. Clegg, S. L., Brimblecombe, P., and Wexler, A. S.: A thermodynamic model of the HC-NH C 4-SO2 4-NO 3-H2O at tropospheric temperatures, J. Phys. Chem. A, 102, 2137-2154, doi:10.1021/Jp973042r, 1998.
18. Clegg, S. L., Seinfeld, J. H., and Brimblecombe, P.: Thermodynamic modelling of aqueous aerosols containing electrolytes and dissolved organic compounds, J. Aerosol. Sci., 32, 713-738, doi:10.1016/S0021-8502(00)00105-1, 2001.
19. Cosman, L. M., and Bertram, A. K.: Reactive uptake of N2O5 on aqueous H2SO4 solutions coated with 1-component and 2-component monolayers, J. Phys. Chem. A, 112, 4625-4635, doi:10.1021/Jp8005469, 2008.
20. Day, D. A., Takahama, S., Gilardoni, S., and Russell, L. M.: Organic composition of single and submicron particles in different regions of western North America and the eastern Pacific during INTEX-B 2006, Atmos. Chem. Phys., 9, 5433-5446, doi:10.5194/acp-9-5433-2009, 2009.
21. DeCarlo, P. F., Dunlea, E. J., Kimmel, J. R., Aiken, A. C., Sueper, D., Crounse, J., Wennberg, P. O., Emmons, L., Shinozuka, Y., Clarke, A., Zhou, J., Tomlinson, J., Collins, D. R., Knapp, D., Weinheimer, A. J., Montzka, D. D., Campos, T., and Jimenez, J. L.: Fast airborne aerosol size and chemistry measurements above Mexico City and Central Mexico during the MILAGRO campaign, Atmos. Chem. Phys., 8, 4027-4048, doi:10.5194/acp-8-4027-2008, 2008.
22. Decesari, S., Fuzzi, S., Facchini, M. C., Mircea, M., Emblico, L., Cavalli, F., Maenhaut, W., Chi, X., Schkolnik, G., Falkovich, A., Rudich, Y., Claeys, M., Pashynska, V., Vas, G., Kourtchev, I., Vermeylen, R., Hoffer, A., Andreae, M. O., Tagliavini, E., Moretti, F., and Artaxo, P.: Characterization of the organic composition of aerosols from Rondônia, Brazil, during the LBASMOCC 2002 experiment and its representation through model compounds, Atmos. Chem. Phys., 6, 375-402, doi:10.5194/acp-6-375-2006, 2006.
23. Dibb, J. E., Talbot, R. W., Klemm, K. I., Gregory, G. L., Singh, H. B., Bradshaw, J. D., and Sandholm, S. T.: Asian influence over the western North Pacific during the fall season: Inferences from lead 210, soluble ionic species and ozone, J. Geophys. Res., 101, 1779-1792, doi:10.1029/94JD03117, 1996.
24. Dibb, J. E., Talbot, R.W., and Scheuer, E. M.: Composition and distribution of aerosols over the North Atlantic during the Subsonic Assessment Ozone and Nitrogen Oxide Experiment (SONEX), J. Geophys. Res., 105, 3709-3717, doi:10.1029/1999JD900424, 2000.
25. Drozd, G. T., Woo, J. L., and McNeill, V. F.: Self-limited uptake of-pinene oxide to acidic aerosol: the effects of liquid-liquid phase separation and implications for the formation of secondary organic aerosol and organosulfates from epoxides, Atmos. Chem. Phys., 13, 8255-8263, doi:10.5194/acp-13-8255-2013, 2013.
26. Erdakos, G. B., Chang, E. I., Pankow, J. F., and Seinfeld, J. H.: Prediction of activity coefficients in liquid aerosol particles containing organic compounds, dissolved inorganic salts, and water-Part 3: Organic compounds, water, and ionic constituents by consideration of short-, mid-, and long-range effects using X-UNIFAC.3, Atmos. Environ., 40, 6437-6452, doi:10.1016/j.atmosenv.2006.04.001, 2006.
27. Escoreia, E. N., Sjostedt, S. J., and Abbatt, J. P. D.: Kinetics of N2O5 hydrolysis on secondary organic aerosol and mixed ammonium bisulfate-secondary organic aerosol particles, J. Phys. Chem. A, 114, 13113-13121, doi:10.1021/jp107721v, 2010.
28. Faucher, J. A., Koleske, J. V., Santee, E. R., Stratta, J. J.,Wilson, C. W.: Glass transitions of ethylene oxide polymers, J. Appl. Phys. 37, 3962-3964, 1966.
29. Finlayson-Pitts, B. J. and Pitts, J. N.: Tropospheric air pollution: Ozone, airborne toxics, polycyclic aromatic hydrocarbons, and particles, Science, 276, 1045-1052, doi:10.1126/science.276.5315.1045, 1997.
30. Finlayson-Pitts, B. J. and Pitts, J. N.: Chemistry of the upper and lower atmosphere: theory, experiments and applications, Academic Press, San Diego, California, London, pp. 969, 2000.
31. Folkers, M., Mentel, T. F., and Wahner, A.: Influence of an organic coating on the reactivity of aqueous aerosols probed by the heterogeneous hydrolysis of N2O5, Geophys. Res. Lett., 30, 1644, doi:10.1029/2003GL017168, 2003.
32. Fu, P. Q., Kawamura, K., and Miura, K.: Molecular characterization of marine organic aerosols collected during a round-the-world cruise, J. Geophys. Res., 116, D13302, doi:10.1029/2011jd015604, 2011.
33. Fuzzi, S., Decesari, S., Facchini, M. C., Matta, E., Mircea, M., and Tagliavini, E.: A simplified model of the water soluble organic component of atmospheric aerosols, Geophys. Res. Lett., 28, 4079-4082, doi:10.1029/2001gl013418, 2001.
34. Gao, S., Keywood, M., Ng, N. L., Surratt, J., Varutbamgkul, V., Bahreini, R., Flagan, R. C., and Seinfeld, J. H.: Low-molecularweight and oligomeric components in secondary organic aerosol from the ozonolysis of cycloalkenes and-pinene, J. Phys. Chem. A, 108, 10147-10164, doi:10.1021/jp047466e, 2004.
35. Gaston, C. J., Thornton, J. A., and Ng, N. L.: Reactive uptake of N2O5 to internally mixed inorganic and organic particles: the role of organic carbon oxidation state and inferred organic phase separations, Atmos. Chem. Phys., 14, 5693-5707, doi:10.5194/acp-14-5693-2014, 2014.
36. Gilardoni, S., Liu, S., Takahama, S., Russell, L. M., Allan, J. D., Steinbrecher, R., Jimenez, J. L., De Carlo, P. F., Dunlea, E. J., and Baumgardner, D.: Characterization of organic ambient aerosol during MIRAGE 2006 on three platforms, Atmos. Chem. Phys., 9, 5417-5432, doi:10.5194/acp-9-5417-2009, 2009.
37. Goldstein, A. H. and Galbally, I. E.: Known and unexplored organic constituents in the earth's atmosphere, Environ, Sci, Technol., 41, 1514-1521, doi:10.1021/es072476p, 2007.
38. Greener, J., Gillmor, J. R., and Daly, R. C.: Melt rheology of a class of polyester ionomers, Marcromolecules, 26, 6416-6424, doi:10.1021/ma00076a018, 1993.
39. 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, doi:10.5194/acp-9-5155-2009, 2009.
40. Hamilton, J. F., Webb, P. J., Lewis, A. C., Hopkins, J. R., Smith, S., and Davy, P.: Partially oxidised organic components in urban aerosol using GCXGC-TOF/MS, Atmos. Chem. Phys., 4, 1279-1290, doi:10.5194/acp-4-1279-2004, 2004.
41. Hawkins, L. N., Russell, L. M., Covert, D. S., Quinn, P. K., and Bates, T. S.: Carboxylic acids, sulfates, and organosulfates in processed continental organic aerosol over the southeast Pacific Ocean during VOCALS-REx 2008, J. Geophys. Res., 115, D13201, doi:10.1029/2009jd013276, 2010.
42. Heald, C. L., Kroll, J. H., Jimenez, J. L., Docherty, K. S., DeCarlo, P. F., Aiken, A. C., Chen, Q., Martin, S. T., Farmer, D. K., and Artaxo, P.: A simplified description of the evolution of organic aerosol composition in the atmosphere, Geophys. Res. Lett., 37, L08803, doi:10.1029/2010gl042737, 2010.
43. Huebert, B. J., Howell, S. G., Zhuang, L., Heath, J. A., Litchy, M. R., Wylie, D. J., Kreidler-Moss, J. L., Coppicus, S., and Pfeiffer, J. E.: Filter and impactor measurements of anions and cations during the First Aerosol Characterization Experiment (ACE 1), J. Geophys. Res., 103, 16493-16509, doi:10.1029/98jd00770, 1998.
44. 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, doi:10.1126/science.1180353, 2009.
45. Kalberer, M., Paulsen, D., Sax, M., Steinbrecher, M., Dommen, J., Prevot, A. S. H., Fisseha, R., Weingartner, E., Frankevich, V., Zenobi, R., and Baltensperger, U.: Identification of ploymers as major components of atmospheric organic aerosols, Science, 303, 1659-1662, doi:10.1126/science.1092185, 2004.
46. Kidd, C., Perraud, V., Wingen, L. M., and Finlayson-Pitts, B. J.: Integrating phase and composition of secondary organic aerosol from the ozonolysis of-pinene, P. Natl. Acad. Sci. USA, 111, 7552-7557, doi:10.1073/pnas.1322558111, 2014.
47. Koop, T., Kapilashrami, A., Molina, L. T., and Molina, M. J.: Phase transitions of sea-salt/water mixtures at low temperatures: Implications for ozone chemistry in the polar marine boundary layer, J. Geophys. Res., 105, 26393-26402, doi:10.1029/2000jd900413, 2000.
48. Koop, T., Bookhold, J., Shiraiwa, M., and Pöschl, U.: Glass transition and phase state of organic compounds: dependency on molecular properties and implications for secondary organic aerosols in the atmosphere, Phys. Chem. Chem. Phys., 13, 19238-19255, doi:10.1039/C1cp22617g, 2011.
49. Krieger, U. K., Marcolli, C., and Reid, J. P.: Exploring the complexity of aerosol particle properties and processes using single particle techniques, Chem. Soc. Rev., 41, 6631-6662, doi:10.1039/C2cs35082c, 2012.
50. Kwamena, N. O. A., Buajarern, J., and Reid, J. P.: Equilibrium Morphology of Mixed Organic/Inorganic/Aqueous Aerosol Droplets: Investigating the Effect of Relative Humidity and Surfactants, J. Phys. Chem. A, 114, 5787-5795, doi:10.1021/jp1003648, 2010.
51. Lee, Y.-N., Weber, R., Ma, Y., Orsini, D., Maxwell-Meier, K., Blake, D., Meinardi, S., Sachse, G., Harward, C., Chen, T. Y., Thornton, D., Tu, F.-H., and Bandy, A.: Airborne measurement of inorganic ionic components of fine aerosol particles using the particle-into-liquid sampler coupled to ion chromatography technique during ACE-Asia and TRACE-P, J. Geophys. Res., 108, 8646, doi:10.1029/2002JD003265, 2003.
52. Levine, I. N.: Physical Chemistry, 6th edition. McGraw-Hill, New York, 2009 Ling, T. Y. and Chan, C. K.: Partical crystallization and deliquescence of particles containing ammonium sulfate and dicarboxylic acids, J. Geophys. Res., 113, D14205, doi:10.1029/2008JD009779, 2008.
53. Liu, S., Takahama, S., Russell, L. M., Gilardoni, S., and Baumgardner, D.: Oxygenated organic functional groups and their sources in single and submicron organic particles in MILAGRO 2006 campaign, Atmos. Chem. Phys., 9, 6849-6863, doi:10.5194/acp-9-6849-2009, 2009.
54. Malcolm, G. N. and Rowlinson, J. S.: The Thermodynamic Properties of Aqueous Solutions of Polyethylene Glycol, Polypropylene Glycol and Dioxane, T. Faraday Soc., 53, 921-931, doi:10.1039/Tf9575300921, 1957.
55. Marcolli, C., and Krieger, U. K.: Phase changes during hygroscopic cycles of mixed organic/inorganic model systems of tropospheric aerosols, J. Phys. Chem. A, 110, 1881-1893, doi:10.1021/jp0556759, 2006.
56. Martin, S. T.: Phase transitions of aqueous atmospheric particles, Chem. Rev., 100, 3403-3453, doi:10.1021/cr990034t, 2000.
57. McNeill, V. F., Patterson, J.,Wolfe, G. M., and Thornton, J. A.: The effect of varying levels of surfactant on the reactive uptake of N2O5 to aqueous aerosol, Atmos. Chem. Phys., 6, 1635-1644, doi:10.5194/acp-6-1635-2006, 2006.
58. Middlebrook, A. M., Murphy, D. M., and Thomson, D. S.: Observations of organic material in individual marine particles at Cape Grim during the First Aerosol Characterization Experiment (ACE 1), J. Geophys. Res., 103, 16475-16483, doi:10.1029/97jd03719, 1998.
59. Mikhailov, E., Vlasenko, S., Martin, S. T., Koop, T., and Pöschl, U.: Amorphous and crystalline aerosol particles interacting with water vapor: conceptual framework and experimental evidence for restructuring, phase transitions and kinetic limitations, Atmos. Chem. Phys., 9, 9491-9522, 2009, http://www.atmos-chem-phys.net/9/9491/2009/.
60. Murphy, D. M. and Thomson, D. S.: Chemical composition of single aerosol particles at Idaho Hill: Negative ion measurements, J. Geophys. Res., 102, 6353-6368, doi:10.1029/96jd00859, 1997.
61. Murphy, D. M., Thomson, D. S., and Mahoney, T. M. J.: In situ measurements of organics, meteoritic material, mercury, and other elements in aerosols at 5 to 19 kilometers, Science, 282, 1664-1669, doi:10.1126/science.282.5394.1664, 1998.
62. Murphy, D. M.: Something in the air, Science, 307, 1888-1890, doi:10.1126/science.1108160, 2005.
63. Murphy, D. M., Cziczo, D. J., Froyd, K. D., Hudson, P. K., Matthew, B. M., Middlebrook, A. M., Peltier, R. E., Sullivan, A., Thomson, D. S., and Weber, R. J.: Single-particle mass spectrometry of tropospheric aerosol particles, J. Geophys. Res., 111, D23S32, doi:10.1029/2006JD007340, 2006.
64. Murray, B. J.: Inhibition of ice crystallisation in highly viscous aqueous organic acid droplets, Atmos. Chem. Phys., 8, 5423-5433, 2008, http://www.atmos-chem-phys.net/8/5423/2008/.
65. 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, doi:10.5194/acp-10-4625-2010, 2010.
66. Nguyen, T. B., Bateman, A. P., Bones, D. L., Nizkorodov, S. A., Laskin, J., and Laskin, A.: High-resolution mass spectrometry analysis of secondary organic aerosol generated by ozonolysis of isoprene, Atmos. Environ., 44, 1032-1042, doi: 10.1016/j.atmosenv.2009.12.019, 2010.
67. Pankow, J. F.: Gas/particle partitioning of neutral and ionizing compounds to single and multi-phase aerosol particles, 1. Unified modeling framework, Atmos. Environ., 37, 3323-3333, doi:10.1016/S1352-2310(03)00346-7, 2003.
68. Pant, A., Fok, A., Parsons, M. T., Mak, J., and Bertram, A. K.: Deliquescence and crystallization of ammonium sulfate-glutaric acid and sodium chloride-glutaric acid particles, Geophys. Res. Lett., 31, L12111, doi:10.1029/2004GL020025, 2004.
69. Pant, A., Parsons, M. T., and Bertram, A. K.: Crystallization of aqueous ammonium sulfate particles internally mixed with soot and kaolinite: Crystallization relative humidities and nucleation rates, J. Phys. Chem. A, 110, 8701-8709, doi:10.1021/jp060985s, 2006.
70. Park, S. C., Burden, D. K., and Nathanson, G. M.: The inhibition of N2O5 hydrolysis in sulfuric acid by 1-butanol and 1-hexanol surfactant coatings, J. Phys. Chem. A, 111, 2921-2929, doi:10.1021/Jp068228h, 2007.
71. Parsons, M. T., Knopf, D. A., and Bertram, A. K.: Deliquescence and crystallization of ammonium sulfate particles internally mixed with water-soluble organic compounds, J. Phys. Chem. A, 108, 11600-11608, doi:10.1021/jp0462862, 2004a.
72. Parsons, M. T., Mak, J., Lipetz, S. R., and Bertram, A. K.: Deliquescence of malonic, succinic, glutaric, and adipic acid particles, J. Geophys. Res., 109, D06212, doi:10.1029/2003JD004075, 2004b.
73. Parsons, M. T., Riffell, J. L., and Bertram, A. K.: Crystallization of aqueous inorganic-malonic acid particles: Nucleation rates, dependence on size, and dependence on the ammonium-to-sulfate, J. Phys. Chem. A, 110, 8108-8115, doi:10.1021/jp057074n, 2006.
74. Pöhlker, C., Wiedemann, K. T., Sinha, B., Shiraiwa, M., Gunthe, S. S., Smith, M., Su, H., Artaxo, P., Chen, Q., Cheng, Y. F., Elbert, W., Gilles, M. K., Kilcoyne, A. L. D., Moffet, R. C., Weigand, M., Martin, S. T., Pöschl, U., and Andreae, M. O.: Biogenic Potassium Salt Particles as Seeds for Secondary Organic Aerosol in the Amazon, Science, 337, 1075-1078, doi:10.1126/science.1223264, 2012.
75. Power, R. M., Simpson, S. H., Reid, J. P., and Hudson, A. J.: The transition from liquid to solid-like behaviour in ultrahigh viscosity aerosol particles, Chem. Sci., 4, 2597-2604, doi:10.1039/C3sc50682g, 2013.
76. Pratt, K. A., and Prather, K. A.: Aircraft measurements of vertical profiles of aerosol mixing states, J. Geophys. Res., 115, D11305, doi:10.1029/2009JD013150, 2010.
77. Prisle, N. L., Engelhart, G. J., Bilde, M., and Donahue, N. M.: Humidity influence on gas-particle phase partitioning of-pinene C O3 secondary organic aerosol, Geophys. Res. Lett., 37, L01802, doi:10.1029/2009GL041402, 2010.
78. Reid, J. P., Dennis-Smither, B. J., Kwamena, N. O. A., Miles, R. E. H., Hanford, K. L., and Homer, C. J.: The morphology of aerosol particles consisting of hydrophobic and hydrophilic phases: hydrocarbons, alcohols and fatty acids as the hydrophobic component, Phys. Chem. Chem. Phys., 13, 15559-15572, doi: 10.1039/c1cp21510h, 2011.
79. Renbaum-Wolff, L., Grayson, J. W., Bateman, A. P., Kuwata, M., Sellier, M., Murray, B. J., Shilling, J. E., Martin, S. T., and Bertram, A. K.: Viscosity of-pinene secondary organic material and implications for particle growth and reactivity, P. Natl. Acad. Sci. USA, 110, 8014-8019, doi:10.1073/pnas.1219548110, 2013.
80. Rogge, W. F., Mazurek, M. A., Hildemann, L. M., Cass, G. R., and Simoneit, B. R. T.: Quantification of urban organic aerosols at a molecular-level: identification, abundance and seasonal-variation, Atmos. Environ. A-Gen, 27, 1309-1330, doi:10.1016/0960-1686(93)90257-Y, 1993.
81. Russell, L. M., Takahama, S., Liu, S., Hawkins, L. N., Covert, D. S., Quinn, P. K., and Bates, T. S.: Oxygenated fraction and mass of organic aerosol from direct emission and atmospheric processing measured on the R/V Ronald Brown during TEXAQS/GoMACCS 2006, J. Geophys. Res., 114, D00F05, doi:10.1029/2008JD011275, 2009.
82. Russell, L. M., Bahadur, R., and Ziemann, P. J.: Identifying organic aerosol sources by comparing functional group composition in chamber and atmospheric particles, P. Natl. Acad. Sci. USA, 108, 3516-3521, doi:10.1073/pnas.1006461108, 2011.
83. Salcedo, D.: Equilibrium phase diagrams of aqueous mixtures of malonic acid and sulfate/ammonium salts, J. Phys. Chem. A, 110, 12158-12165, doi:10.1021/jp063850v, 2006.
84. Saukko, E., Lambe, A. T., Massoli, P., Koop, T., Wright, J. P., Croasdale, D. R., Pedernera, D. A., Onasch, T. B., Laaksonen, A., Davidovits, P., Worsnop, D. R., and Virtanen, A.: Humiditydependent phase state of SOA particles from biogenic and anthropogenic precursors, Atmos. Chem. Phys., 12, 7517-7529, doi:10.5194/acp-12-7517-2012, 2012.
85. Saxena, P. and Hildemann, L. M.: Water-soluble organics in atmospheric particles: A critical review of the literature and application of thermodynamics to identify candidate compounds, J. Atmos. Chem., 24, 57-109, doi:10.1007/BF00053823, 1996.
86. Schill, G. P. and Tolbert, M. A.: Heterogeneous ice nucleation on phase-separated organic-sulfate particles: effect of liquid vs. glassy coatings, Atmos. Chem. Phys., 13, 4681-4695, doi:10.5194/acp-13-4681-2013, 2013.
87. Seinfeld, J. H., Erdakos, G. B., Asher, W. E., and Pankow, J. F.: Modeling the formation of secondary organic aerosol (SOA). 2. The predicted effects of relative humidity on aerosol formation in the-pinene-,-pinene-, sabinene-, 13-Carene-, and cyclohexene-ozone systems, Environ. Sci. Technol., 35, 1806-1817, doi:10.1021/es001765C, 2001.
88. Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics: From Air pollution to Climate Change, 2nd ed., Wiley-Interscience, Hoboken, New Jersey, 2006.
89. Shiraiwa, M., Zuend, A., Bertram, A. K., and Seinfeld, J. H.: Gasparticle partitioning of atmospheric aerosols: interplay of physical state, non-ideal mixing and morphology, Phys. Chem. Chem. Phys., 15, 11441-11453, doi:10.1039/C3cp51595h, 2013.
90. Slade, L. and Levine, H.: Water and the glass-transition-dependence of the glass-transition on composition and chemical-structure-special implications for flour functionality in cookie baking, J. Food Eng., 22, 143-188, doi:10.1016/0260-8774(94)90029-9, 1994.
91. Smith, M. L., Kuwata, M., and Martin, S. T.: Secondary organic material produced by the dark ozonolysis of-pinene minimally affects the deliquescence and efflorescence of ammonium sulfate, Aerosol Sci. Technol., 45, 244-261, doi:10.1080/02786826.2010.532178, 2011.
92. Smith, M. L., Bertram, A. K., and Martin, S. T.: Deliquescence, efflorescence, and phase miscibility of mixed particles of ammonium sulfate and isoprene-derived secondary organic material, Atmos. Chem. Phys., 12, 9613-9628, doi:10.5194/acp-12-9613-2012, 2012.
93. Song, M., Marcolli, C., Krieger, U. K., Zuend, A., and Peter, T.: Liquid-liquid phase separation and morphology of internally mixed dicarboxylic acids/ammonium sulfate/water particles, Atmos. Chem. Phys., 12, 2691-2712, doi:10.5194/acp-12-2691-2012, 2012a.
94. Song, M., Marcolli, C., Krieger, U. K., Zuend, A., and Peter, T.: Liquid-liquid phase separation in aerosol particles: Dependence on O: C, organic functionalities, and compositional complexity, Geophys. Res. Lett., 39, L19801, doi:10.1029/2012GL052807, 2012b.
95. Song, M., Marcolli, C., Krieger, U. K., Lienhard, D. M., and Peter, T.: Morphologies of mixed orgnaic/inorganic/aqueous aerosol droplets, Faraday Discuss., 165, 289-316, doi:10.1039/C3FD00049D, 2013.
96. Takahama, S., Schwartz, R. E., Russell, L. M., Macdonald, A. M., Sharma, A., and Leaitch, W. R.: Organic functional groups in aerosol particles from burning and non-burning forest emissions at high-elevation mountain site, Atmos. Chem. Phys., 11, 6367-6386, doi:10.5194/acp-11-6367-2011, 2011.
97. Talbot, R. W., Dibb, J. E., and Loomis, M. B.: Influence of vertical transport on free tropospheric aerosols over the central USA in springtime, Geophys. Res. Lett., 25, 1367-1370, doi:10.1029/98GL00184, 1998.
98. Thornton, J. A. and Abbatt, J. P. D.: N2O5 reaction on submicron sea salt aerosol: Kinetics, products, and the effect of surface active organics, J. Phys. Chem. A, 109, 10004-10012, doi:10.1021/Jp054183t, 2005.
99. Tolocka, M. P., Jang, M., Ginter, J. M., Cox, R. J., Kamens, R. M., and Johnston, M. V.: Formation of oligomers in secondary organic aerosol, Environ, Sci, Technol., 38, 1428-1434, doi:10.1021/es035030r, 2004.
100. Tolocka, M. P., Lake, D. A., Johnston, M. V., and Wexler, A. S.: Size-resolved fine and ultrafine particle composition in Baltimore, Maryland, J. Geophys. Res., 110, D07S04, doi:10.1029/2004JD004573, 2005.
101. Tong, H. J., Reid, J. P., Bones, D. L., Luo, B. P., and Krieger, U. K.: Measurements of the timescales for the mass transfer of water in glassy aerosol at low relative humidity and ambient temperature, Atmos. Chem. Phys., 11, 4739-4754, doi:10.5194/acp-11-4739-2011, 2011.
102. Treuel, L., Pederzani, S., and Zellner, R.: Deliquescence behaviour and crystallisation of ternary ammonium sulfate/dicarboxylic acid/water aerosols, Phys. Chem. Chem. Phys., 11, 7976-7984, doi:10.1039/b905007h, 2009.
103. Veghte, D. P., Altaf, M. B., and Freedman, M. A.: Size Dependence of the Structure of Organic Aerosol, J. Am. Chem. Soc., 135, 16046-16049, doi:10.1021/Ja408903g, 2013.
104. Veghte, D. P., Bittner, D. R., and Freedman, M. A.: Cryo-Transmission Electron Microscopy Imaging of the Morphology of Submicrometer Aerosol Containing Organic Acids and Ammonium Sulfate, Anal. Chem., 86, 2436-2442, doi:10.1021/ac403279f, 2014.
105. Wise, M. E., Surratt, J. D., Curtis, D. B., Shilling, J. E., and Tolbert, M. A.: Hygroscopic growth of ammonium sulfate/dicarboxylic acids, J. Geophys. Res., 108, 4638, doi:10.1029/2003JD003775, 2003.
106. You, Y., Renbaum-Wolff, L., Carreras-Sospedra, M., Hanna, S. J., Hiranuma, N., Kamal, S., Smith, M. L., Zhang, X. L., Weber, R. J., Shilling, J. E., Dabdub, D., Martin, S. T., and Bertram, A. K.: Images reveal that atmospheric particles can undergo liquidliquid phase separations, P. Natl. Acad. Sci. USA, 109, 13188-13193, doi:10.1073/pnas.1206414109, 2012.
107. You, Y., Renbaum-Wolff, L., and Bertram, A. K.: Liquid-liquid phase separation in particles containing organics mixed with ammonium sulfate, ammonium bisulfate, ammonium nitrate or sodium chloride, Atmos. Chem. Phys., 13, 11723-11734, doi:10.5194/acp-13-11723-2013, 2013.
108. You, Y., Smith, M. L., Song, M., Martin, S. T., and Bertram, A. K.: Liquid-liquid phase separation in atmospherically relevant parti- cles consisting of organic species and inorganic salts, Int. Rev. Phys. Chem., 33, 43-77, doi:10.1080/0144235X.2014.890786, 2014.
109. Zobrist, B., Marcolli, C., Pedernera, D. A., and Koop, T.: Do atmospheric aerosols form glasses?, Atmos. Chem. Phys., 8, 5221-5244, 2008, http://www.atmos-chem-phys.net/8/5221/2008/.
110. Zobrist, B., Soonsin, V., Luo, B. P., Krieger, U. K., Marcolli, C., Peter, T., and Koop, T.: Ultra-slow water diffusion in aqueous sucrose glasses, Phys. Chem. Chem. Phys., 13, 3514-3526, doi:10.1039/c0cp01273d, 2011.
111. Zuend, A., Marcolli, C., Luo, B. P., and Peter, T.: A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients, Atmos. Chem. Phys., 8, 4559-4593, doi:10.5194/acp-8-4559-2008, 2008.
112. Zuend, A., Marcolli, C., Peter, T., and Seinfeld, J. H.: Computation of liquid-liquid equilibria and phase stabilities: implications for RH-dependent gas/particle partitioning of organic-inorganic aerosols, Atmos. Chem. Phys., 10, 7795-7820, doi:10.5194/acp-10-7795-2010, 2010.
113. Zuend, A., Marcolli, C., Booth, A. M., Lienhard, D. M., Soonsin, V., Krieger, U. K., Topping, D. O., McFiggans, G., Peter, T., and Seinfeld, J. H.: New and extended parameterization of the thermodynamic model AIOMFAC: calculation of activity coefficients for organic-inorganic mixtures containing carboxyl, hydroxyl, carbonyl, ether, ester, alkenyl, alkyl, and aromatic functional groups, Atmos. Chem. Phys., 11, 9155-9206, doi:10.5194/acp-11-9155-2011, 2011.
114. Zuend, A. and Seinfeld, J. H.: Modeling the gas-particle partitioning of secondary organic aerosol: the importance of liquidliquid phase separation, Atmos. Chem. Phys., 12, 3857-3882, doi:10.5194/acp-12-3857-2012, 2012.
115. Zuend, A. and Seinfeld, J. H.: A practical method for the calculation of liquid-liquid equilibria in multicomponent organic-waterelectrolyte systems using physicochemical constraints, Fluid Phase Equilib., 337, 201-213, doi:10.1016/j.fluid.2012.09.034, 2013.