References

ACPD

Atmospheric Chemistry and Physics Discussions

ACPD

1680-7375

Copernicus GmbH

Göttingen, Germany

10.5194/acpd-11-12441-2011

Microphysical simulations of new particle formation in the upper troposphere and lower stratosphere

English

J. M.

¹ Toon

O. B.

¹ Mills

M. J.

² Yu

Laboratory for Atmospheric and Space Physics, Department of Atmospheric and Oceanic Sciences, University of Colorado, Boulder, CO, USA

NCAR Earth System Laboratory, National Center for Atmospheric Research, Boulder, CO, USA

Atmospheric Sciences Research Center, State University of New York, Albany, NY, USA

20 04 2011

11 4 12441 12486

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-discuss.net/11/12441/2011/acpd-11-12441-2011.html

The full text article is available as a PDF file from http://www.atmos-chem-phys-discuss.net/11/12441/2011/acpd-11-12441-2011.pdf

Using a three-dimensional general circulation model with sulfur chemistry and sectional aerosol microphysics (WACCM/CARMA), we studied aerosol formation and microphysics in the tropical upper troposphere and lower stratosphere (UTLS) based on three nucleation schemes (two binary homogeneous schemes and an ion-mediated scheme). Simulations suggest that ion-mediated nucleation rates in the UTLS are 25% higher than binary rates, but that the rates predicted by the two binary schemes vary by two orders of magnitude. However, it is found that coagulation, not nucleation, controls number concentration at sizes greater than approximately 10 nm. Therefore, based on this study, atmospherically relevant processes in the UTLS are not sensitive to the choice of nucleation schemes. The dominance of coagulation over other microphysical processes is consistent with other recent work using microphysical models. Simulations using all three nucleation schemes compare reasonably well to observations of size distributions, number concentration across latitude, and vertical profiles of particle mixing ratio in the UTLS. Interestingly, we find we need to include Van der Waals forces in our coagulation scheme to match the UTLS aerosol concentrations. We conclude that this model can accurately represent sulfate microphysical processes in the UTLS, and that the properties of particles at atmospherically relevant sizes are not sensitive to the details of the nucleation scheme. We also suggest that micrometeorites, which are not included in this model, dominate the aerosol properties in the upper stratosphere above about 30 km.

References 1

Alam, M. K.: The effect of Van der Waals and viscous forces on aerosol coagulation, Aerosol Sci. Tech., 6(1), 41–52, http://dx.doi.org/10.1080/02786828708959118doi:10.1080/02786828708959118, 1987.

Arnold, F., Fabian, R., and Joos, W.: Measurements of the height variation of sulfuric-acid vapor concentrations in the stratosphere, Geophys. Res. Lett., 8, 293–296, 1981.

Ayers, G. P., Gillett, R. W., and Gras, J. L.: On the vapor-pressure of sulfuric acid, Geophys. Res. Lett., 7(6), 433–436, 1980.

Bardeen, C. G., Toon, O. B., Jensen, E. J., Marsh, D. R., and Harvey, V. L.: Numerical simulations of the three-dimensional distribution of meteoric dust in the mesosphere and upper stratosphere, J. Geophys. Res., 113, D17202, http://dx.doi.org/10.1029/2007jd009515doi:10.1029/2007jd009515, 2008.

Bardeen, C. G., Toon, O. B., Jensen, E. J., Hervig, M. E., Randall, C. E., Benze, S., Marsh, D. R., and Merkel, A.: Numerical simulations of the three-dimensional distribution of polar mesospheric clouds and comparisons with Cloud Imaging and Particle Size (CIPS) experiment and the Solar Occultation For Ice Experiment (SOFIE) observations, J. Geophys. Res., 115, D10204, http://dx.doi.org/10.1029/2009JD012451doi:10.1029/2009JD012451, 2010.

Barth, M. C., Rasch, P. J., Kiehl, J. T., Benkovitz, C. M., and Schwartz, S. E.: Sulfur chemistry in the National Center for Atmospheric Research Community Climate Model: Description, evaluation, features, and sensitivity to aqueous chemistry, J. Geophys. Res.-Atmos., 105(D1), 1387–1415, 2000.

Bates, T. S., Huebert, B., Gras, J., Griffiths, F., and Durkee, P.: The International Global Atmospheric Chemistry (IGAC) Project's First Aerosol Characterization Experiment (ACE-1): Overview, J. Geophys. Res., 103, 16297–16318, 1998.

Blitz, M. A., McKee, K. W., and Pilling, M. J.: Temperature dependence of the reaction of OH with SO, P. Combust. Inst., 28, 2491–2497, 2000.

Blitz, M. A., Hughes, K. J., and Pilling, M. J.: Determination of the high-pressure limiting rate coefficient and the enthalpy of reaction for OH+SO2, J. Phys. Chem. A, 101, 1971–1978, 2003.

Borrmann, S., Kunkel, D., Weigel, R., Minikin, A., Deshler, T., Wilson, J. C., Curtius, J., Volk, C. M., Homan, C. D., Ulanovsky, A., Ravegnani, F., Viciani, S., Shur, G. N., Belyaev, G. V., Law, K. S., and Cairo, F.: Aerosols in the tropical and subtropical UT/LS:~in-situ measurements of submicron particle abundance and volatility, Atmos. Chem. Phys., 10, 5573–5592, http://dx.doi.org/10.5194/acp-10-5573-2010doi:10.5194/acp-10-5573-2010, 2010.

Brock, C. A., Hamill, P., Wilson, J. C., Jonsson, H. H., and Chan, K. R.: Particle formation in the upper tropical troposphere – A source of nuclei for the stratospheric aerosol, Science, 270, 1650–1653, 1995.

Brunning, J. and Stief, L. J.: Kinetic studies of the reaction of the SO radical with NO2 and ClO from 210 to 363 K, J. Chem. Phys., 84, 4371–4377, 1986a.

Brunning, J. and Stief, L. J.: Rate constant for the reaction SO + BrO -> SO2 + Br, J. Chem. Phys., 85(5), 2591, http://dx.doi.org/10.1063/1.451066doi:10.1063/1.451066, 1986b.

Burkholder, J. B. and McKeen, S.: UV absorption cross-section for SO3, Geophys. Res. Lett., 24(24), 3201–3204, 1997.

Chan, T. W. and Mozurkewich, M.: Measurement of the coagulation rate constant for sulfuric acid particles as a function of particle size using tandem differential mobility analysis, J. Aerosol Sci., 32(3), 321–339, 2001.

Cheng, B. M. and Lee, Y. P.: Rate constant of OH + OCS reaction over the temperature range 255–483 K, Int. J. Chem. Kinet., 18, 1303–1314, 1986.

Chu, W. P., McCormick, M. P., Lenoble, J., Brogniez, C., and Pruvost, P.: SAGE II inversion algorithm, J. Geophys. Res., 94, 8339–8351, 1989.

Clarke, A. D.: Atmospheric nuclei in the Pacific midtroposphere – their nature, concentration, and evolution, J. Geophys. Res.-Atmos., 98(D11), 20633–20647, 1993.

Clarke, A. D. and Kapustin, V. N.: A Pacific aerosol survey. part I: A decade of data on particle production, transport, evolution, and mixing in the troposphere, J. Atmos. Sci., 52, 363–382, 2002.

Clyne, M. A. A. and MacRobert, A. J.: Kinetic-studies of free-radical reactions by mass-spectrometry, Int. J. Chem. Kinet., 13, 187–197, 1981.

Clyne, M. A. A. and Townsend, L. W.: Rate constant measurements for rapid reactions of ground-state sulfur 3P4(P-3(J)) atoms, Int. J. Chem. Kinet., Symp. 1, 73–84, 1975.

Coffman, D. J. and Hegg, D. A.: A preliminary study of the effect of ammonia on particle nucleation in the marine boundary layer, J. Geophys. Res., 100(D4), 7147–7160, 1995.

Colella, P. and Woodward, P. R.: The piecewise parabolic method (PPM) for gas-dynamical simulations, J. Comput. Phys., 54(1), 174–201, 1984.

Crutzen, P. J.: Albedo enhancement by stratospheric sulfur injections: A contribution to resolve a policy dilemma?, Climatic Change, 77(3–4), 211–219, 2006.

Curtius, J., Sierau, B., Arnold, F., de Reus, M., Strom, J., Scheeren, H. A., and Lelieveld, J.: Measurement of aerosol sulfuric acid 2. Pronounced layering in the free troposphere during the second Aerosol Characterization Experiment (ACE 2), J. Geophys. Res.-Atmos., 106(D23), 31975–31990, 2001.

Davis, D. D., Klemm, R. B. and Pilling, M.: A flash photolysis-resonance fluorescence kinetics study of ground-state sulfur atoms: I. Absolute rate parameters for reaction of S(3P) with O$_2(^3§igma )$, Int. J. Chem. Kinet., 4, 367–382, http://dx.doi.org/10.1002/kin.550040402doi:10.1002/kin.550040402, 1972.

Deshler, T., Hervig, M. E., Hofmann, D. J., Rosen, J. M., and Liley, J. B.: Thirty years of in-situ stratospheric aerosol size distribution measurements from Laramie, Wyoming (41N), using balloon-borne instruments, J. Geophys. Res., 108(D5), 4167, http://dx.doi.org/10.1029/2002JD002514doi:10.1029/2002JD002514, 2003.

Eisele, F. L., Lovejoy, E. R., Kosciuch, E., Moore, K. F., Mauldin III, R. L., Smith, J. N., McMurry, P. H., and Iida, K.: Negative atmospheric ions and their potential role in ion-induced nucleation, J. Geophys. Res., 111, D04305, http://dx.doi.org/10.1029/2005JD006568doi:10.1029/2005JD006568, 2006.

Fan, T. and Toon, O. B.: Modeling sea-salt aerosol in a coupled climate and sectional microphysical model: mass, optical depth and number concentration, Atmos. Chem. Phys. Discuss., 10, 24499–24561, http://dx.doi.org/10.5194/acpd-10-24499-2010doi:10.5194/acpd-10-24499-2010, 2010.

Flood, H.: Droplet formation in oversaturated ethanol-water vapour mixtures, Zeit. Chem. Phys., 170(3/4), 286–294, 1934.

Fuchs, N. A.: The Mechanics of Aerosols, Pergamon, New York, 1964.

Garcia, R. R, Marsh, D. R., Kinnison, D. E., Boville, B. A., and Sassi, F.: Simulation of secular trends in the middle atmosphere, 1950–2003, J. Geophys. Res.-Atmos., 112(D9), D09301, http://dx.doi.org/10.1029/2006JD007485doi:10.1029/2006JD007485, 2007.

Giauque, W. F., Hornung, E. W., Kunzler, J. E., and Rubin, T. R.: The thermodynamic properties of aqueous sulfuric acid solutions and hydrates from 15-degrees-K to 300-degrees-K, J. Amer. Chem. Soc., 82(10), 62–70, 1960.

Hamill, P., Toon, O. B., and Kiang, C. S.: Microphysical processes affecting stratospheric aerosol particles, J. Atmos. Sci., 34, 1104–1119, 1977.

Hanson, D. R. and Lovejoy, E. R.: Measurement of the thermodynamics of the hydrated dimer and trimer of sulfuric acid, J. Phys. Chem. A-Letters, 110, 9525–9528, 2006.

Heckendorn, P., Weisenstein, D., Fueglistaler, S., Luo, B. P., Rozanov, E. Schraner, M., Thomason, L. W., and Peter, T.: The impact of geoengineering aerosols on stratospheric temperature and ozone, Environ. Res. Lett., 4, 045108, http://dx.doi.org/10.1088/1748-9326/4/4/045108doi:10.1088/1748-9326/4/4/045108, 2009.

Heintzenberg, J., Hermann, M., and Theiss, D.: Out of Africa: High aerosol concentrations in the upper troposphere over Africa, Atmos. Chem. Phys., 3, 1191–1198, http://dx.doi.org/10.5194/acp-3-1191-2003doi:10.5194/acp-3-1191-2003, 2003.

Hervig, M. E., Gordley, L. L., Deaver, L. E., Siskind, D. E., Stevens, M. H., Russell III, J. M., Bailey, S. M., Megner, L., and Bardeen, C. G.: First satellite observations of meteoric smoke in the middle atmosphere, Geophys. Res. Lett., 36, L18805, http://dx.doi.org/10.1029/2009GL039737doi:10.1029/2009GL039737, 2009.

Hoell, J. M., Davis, D. D., Jacob, D. J., Rodgers, M. O., Newell, R. E., Fuelberg, H. E., McNeal, R. J., Raper, J. L., and Bendura, R. J.: Pacific Exploratory Mission in the tropical Pacific: PEM-Tropics A, August–September 1996, J. Geophys. Res., 104(D5), 5567–5583, 1999.

Hofman, D. J. and Solomon, S.: Ozone destruction through heterogeneous chemistry following the eruption of El Chichon, J. Geophys. Res.-Atmos., 94(D4), 5029–5041, 1989.

Huang, D. D., Seinfeld, J. H., and Marlow, W. H.: BGK equation solution of coagulation for large Knudsen number aerosols with a singular attractive contact potential, J. Colloid Interf. Sci., 140(1), 258–276, http://dx.doi.org/10.1016/0021-9797(90)90341-Kdoi:10.1016/0021-9797(90)90341-K, 1990.

Hunten, M. D., Turco, R. P., and Toon, O. B.: Smoke and dust particles of meteoric origin in the mesosphere and stratosphere, J. Atmos. Sci., 37, 1342–1357, 1980.

Jensen, E. J., Toon, O. B., Selkirk, H. B., Spinhirne, J. D., and Schoeberl, M. R.: On the formation and persistence of subvisible cirrus clouds near the tropical tropopause, J. Geophys. Res., 101(D16), 21361–21375, 1996.

Jourdain, J. L., Le Bras, G., and Combourieu, J.: Kinetic study of reactions of 1,1,1 trifluoro-2 chloroethane with chlorine atoms and oxygen atoms, J. Chim. Phys., 75, 318–323, 1978.

Kanawade, V. and Tripathi, S. N.: Evidence for the role of ion-induced particle formation during an atmospheric nucleation event observed in Tropospheric Ozone Production about the Spring Equinox (TOPSE), J. Geophys. Res.-Atmos., 111(D2), D02209, http://dx.doi.org/10.1029/2005JD006366doi:10.1029/2005JD006366, 2006.

Kazil, J., Lovejoy, E. R., Jensen, E. J., and Hanson, D. R.: Is aerosol formation in cirrus clouds possible?, Atmos. Chem. Phys., 7, 1407–1413, http://dx.doi.org/10.5194/acp-7-1407-2007doi:10.5194/acp-7-1407-2007, 2007.

Kazil, J., Stier, P., Zhang, K., Quaas, J., Kinne, S., O'Donnell, D., Rast, S., Esch, M., Ferrachat, S., Lohmann, U., and Feichter, J.: Aerosol nucleation and its role for clouds and Earth's radiative forcing in the aerosol-climate model ECHAM5-HAM, Atmos. Chem. Phys., 10, 10733–10752, http://dx.doi.org/10.5194/acp-10-10733-2010doi:10.5194/acp-10-10733-2010, 2010.

Kinnison, D. E., Brasseur, G. P., Walters, S., Garcia, R. R., Marsh, D. R., Sassi, F., Harvey, V. L., Randall, C. E., Emmons, L., Lamarque, J. F., Hess, P., Orlando, J. J., Tie, X. X., Randel, W., Pan, L. L, Gettelman, A., Granier, C., Diehl, T., Niemeier, U., and Simmons, A. J.: Sensitivity of chemical tracers to meteorological parameters in the MOZART-3 chemical transport model, J. Geophys. Res., 112, D20302, http://dx.doi.org/10.1029/2006JD007879doi:10.1029/2006JD007879, 2007.

Kulmala, M. and Laaksonen, A.: Binary nucleation of water sulfuric-acid system – comparison of classical-theories with different H2SO4 saturation vapor-pressures, J. Chem. Phys., 93(1), 696–701, 1990.

Lamarque J.-F., Bond, T. C., Eyring, V., Granier, C., Heil, A., Klimont, Z., Lee, D., Liousse, C., Mieville, A., Owen, B., Schultz, M. G., Shindell, D., Smith, S. J., Stehfest, E., Van Aardenne, J., Cooper, O. R., Kainuma, M., Mahowald, N., McConnell, J. R., Naik, V., Riahi, K., and van Vuuren, D. P.: Historical (1850–2000) gridded anthropogenic and biomass burning emissions of reactive gases and aerosols: methodology and application, Atmos. Chem. Phys., 10(15), 7017–7039, 2010.

Lee, S.-H., Reeves, J. M., Wilson, J. C., Hunton, D. E., Viggiano, A. A., Miller, T. M., Ballenthin, J. O., and Lait, L. R.: Particle formation by ion induced nucleation in the upper troposphere and lower stratosphere, Science, 301, 1886–1889, 2003.

Lin, S. J. and Rood, R. B: Multidimensional flux-form semi-Lagrangian transport schemes, Mon. Weather Rev., 124(9), 2046–2070, 1996.

Lin, S. J. and Rood, R. B.: An explicit flux-form semi-Lagrangian shallow-water model on the sphere, Q. J. Roy. Meteorol. Soc., 123, 2477–2498, 1997.

Lin, J. S. and Tabazadeh, A.: A parameterization of an aerosol physical chemistry model for the NH3/H2SO4/HNO3/H2O system at cold temperatures, J. Geophys. Res.-Atmos., 106(D5), 4815–4829, 2001.

Lovejoy, E. R., Hanson, D. R., and Huey, L. G.: Kinetics and products of the gas-phase reaction of SO3 with water, J. Phys. Chem., 100(51), 19911–19916, 1996.

Lovejoy, E. R., Curtius, J., and Froyd, K. D.: Atmospheric ion-induced nucleation of sulfuric acid and water, J. Geophys. Res., 109, D08204, http://dx.doi.org/10.1029/2003JD004460doi:10.1029/2003JD004460, 2004.

Lucas, D. D. and Prinn, R. G.: Tropospheric distributions of sulfuric acid-water vapor aerosol nucleation rates from dimethylsulfide oxidation, Geophys. Res. Lett., 30(22), 2136, http://dx.doi.org/10.1029/2003GL018370doi:10.1029/2003GL018370, 2003.

Mills, M. J., Toon, O. B., Turco, R. P., Kinnison, D. E., and Garcia, R. R.: Massive global ozone loss predicted following regional nuclear conflict, PNAS, 105(14), 5307–5312, http://dx.doi.org/10.1073/pnas.0710058105doi:10.1073/pnas.0710058105, 2008.

Molina, L. T. and Molina, M. J.: UV absorption cross-sections of HO2NO2 vapor, J. Photochem., 15, 97–108, 1981.

Okabe, H.: In Photochemistry of Small Molecules, John Wiley and Sons Inc., New York, 248–249, 1978.

Palmer, K. F. and Williams, D.: Optical constants of sulfuric acid; Application to the clouds of Venus?, Appl. Optics, 14, 208–219, 1975.

Pierce, J. R. and Adams, P. J.: Efficiency of cloud condensation nuclei formation from ultrafine particles, Atmos. Chem. Phys., 7, 1367–1379, http://dx.doi.org/10.5194/acp-7-1367-2007doi:10.5194/acp-7-1367-2007, 2007.

Pierce, J. R. and Adams, P. J.: Can cosmic rays affect cloud condensation nuclei by altering new particle formation rates?, Geophys. Res. Lett., 36, L09820, http://dx.doi.org/10.1029/2009GL037946doi:10.1029/2009GL037946, 2009.

Rasch, P. J., Tilmes, S., Turco, R. P., Robock, A., Oman, L., Chen, C., Stenchikov, G. L., and Garcia, R. R.: An overview of geoengineering of climate using stratospheric sulphate aerosols, Philos. T. R. Soc. A, 366(1882), 4007–4037, 2008.

Reiner, T. and Arnold, F.: Stratospheric SO3: Upper limits inferred from ion composition measurement: Implications for H2SO4 and aerosol formation, Geophys. Res. Lett., 24, 1751–1754, 1997.

Reiss, H.: The kinetics of phase transitions in binary systems, J. Chem. Phys., 18(6), 840–848, 1950.

Robock, A., Oman, L., and Stenchikov, G. L.: Regional climate responses to geoengineering with tropical and Arctic SO2 injections, J. Geophys. Res.-Atmos., 113, D16101, http://dx.doi.org/10.1029/2008JD010050doi:10.1029/2008JD010050, 2008.

Ross, M., Mills, M., and Toohey, D.: Potential climate impact of black carbon emitted by rockets, Geophys. Res. Lett., 37, L24810, http://dx.doi.org/10.1029/2010GL044548doi:10.1029/2010GL044548, 2010.

Sabinina, A. L. and Terpugow, L.: Die oberflachenspannung de systems schwefelsaure-wasser, Z. Phys. Chem. A, 173, 237–241, 1935.

Sander, S. P., Finlayson-Pitts, B. J., Friedl, R. R., Golden, D. M., Huie, R. E., Keller-Rudek, H., Kolb, C. E., Kurylo, M. J., Molina, M. J., Moortgat, G. K., Orkin, V. L., Ravishankara, A. R., and Wine, P. H.: Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies, Evaluation Number 15, JPL Publication 06-2, Jet Propulsion Laboratory, Pasadena, 2006.

Schlager, H. and Arnold, F.: Balloon-borne composition measurements of stratospheric negative-ions and inferred sulfuric-acid vapor abundances during the Map-Globus 1983 campaign, Planet. Space Sci., 35, 693–701, 1987.

Schmidt-Ott, A. and Burtscher, H.: The effect of Van der Waals forces on aerosol coagulation, J. Colloid Interf. Sci., 89(2), 353–357, http://dx.doi.org/10.1016/0021-9797(82)90187-4doi:10.1016/0021-9797(82)90187-4, 1982.

Smith, S. J., van Aardenne, J., Klimont, Z., Andres, R. J., Volke, A., and Delgado Arias, S.: Anthropogenic sulfur dioxide emissions: 1850-2005, Atmos. Chem. Phys., 11, 1101–1116, http://dx.doi.org/10.5194/acp-11-1101-2011doi:10.5194/acp-11-1101-2011, 2011.

Su, L. and Toon, O. B.: Saharan and asian dust: similarities and differences determined by CALIPSO, AERONET and a coupled climate-aerosol microphysical model, Atmos. Chem. Phys. Discuss., 10, 29513–29567, http://dx.doi.org/10.5194/acpd-10-29513-2010doi:10.5194/acpd-10-29513-2010, 2010.

Tabazadeh, A., Toon, O. B., Clegg, S. L., and Hamill, P.: A new parameterization of H2SO4/H2O aerosol composition: Atmospheric implications. Geophys. Res. Lett., 24(15), 1931–1934, 1997.

Thornton, D. C., Bandy, A. R., Blomquist, B. W., Driedger, A. R., and Wade, T. P.: Sulfur dioxide distribution over the Pacific Ocean 1991–1996, J. Geophys. Res., 104, 5845–5854, 1999.

Timmreck, C., Graf, H.-F., Lorenz, S. J., Niemeier, U., Zanchettin, D., Matei, D., Jungclaus, J. H., and Crowley, T. J.: Aerosol size confines climate response to volcanic super-eruptions, Geophys. Res. Lett., 37, L24705, http://dx.doi.org/10.1029/2010GL045464doi:10.1029/2010GL045464, 2010.

Toon, O. B., Turco, R. P., Westphal, D., Malone, R., and Liu, M. S.: A multidimensional model for aerosols – description of computational analogs, J. Atmos. Sci., 45, 2123–2143, 1988.

Usoskin, I. G., Desorgher, L., Velinov, P., Storini, M., Fluckiger, E. O., Butikofer, R., and Kovaltsov, G. A.: Ionization of the earth's atmosphere by solar and galactic cosmic rays, Acta Geophys., 57(1), 88–101, 2009.

Vaida, V., Kjaergaard, H. G., Hintze, P. E., and Donaldson, D. J.: Photolysis of sulfuric acid vapor by visible solar radiation, Science, 299, 1566–1568, 2003.

Viggiano, A. A. and Arnold, F.: Extended sulfuric acid vapor concentration measurements in the stratosphere, Geophys. Res. Lett., 8, 583–586, 1981.

Wang, P. H., Minnis, P., and Yue, G. K.: Extinction coefficient (1 um) properties of high-altitude clouds from solar occultation measurements (1985–1990): Evidence of volcanic aerosol effect, J. Geophys. Res., 100(D2), 3181–3199, 1995.

Wang, P. H., Kent, G. S., and McCormick, M. P.: Retrieval analysis of aerosol-size distribution with simulated extinction measurements at SAGE III wavelengths, Appl. Opt., 35(3), 433–440, 1996.

Wang, Y. H., Liu, S. C., Wine, P. H., Davis, D. D., Sandholm, S. T., Atlas, E. L., Avery, M. A., Blake, D. R., Blake, N. J., Brune, W. H., Heikes, B. G., Sachse, G. W., Shetter, R. E., Singh, H. B., Talbot, R. W., and Tan, D.: Factors controlling tropospheric O-3, OH, NOx and SO2 over the tropical Pacific during PEM-Tropics B, J. Geophys. Res.-Atmos., 106(D23), 32733–32747, 2001.

Wilson, J. C., Lee, S.-H., Reeves, J. M., Brock, C. A., Jonsson, H. H., Lafleur, B. G., Loewenstein, M., Podolske, J., Atlas, E., Boering, K., Toon, G., Fahey, D., Bui, T. P., Diskin, G., and Moore, F.: Steady-state aerosol distributions in the extra-tropical, lower stratosphere and the processes that maintain them, Atmos. Chem. Phys., 8, 6617–6626, http://dx.doi.org/10.5194/acp-8-6617-2008doi:10.5194/acp-8-6617-2008, 2008.

Yu, F.: Updated H2SO4-H2O binary homogeneous nucleation look-up tables, J. Geophys. Res., 113, D24201, http://dx.doi.org/10.1029/2008JD010527doi:10.1029/2008JD010527, 2008.

Yu, F.: Ion-mediated nucleation in the atmosphere: Key controlling parameters, implications, and look-up table, J. Geophys. Res., 115, D03206, http://dx.doi.org/10.1029/2009JD012630doi:10.1029/2009JD012630, 2010.

Yu, F. and Luo, G.: Simulation of particle size distribution with a global aerosol model: contribution of nucleation to aerosol and CCN number concentrations, Atmos. Chem. Phys., 9, 7691–7710, http://dx.doi.org/10.5194/acp-9-7691-2009doi:10.5194/acp-9-7691-2009, 2009.

Yu, F. and Turco, R. P.: From molecular clusters to nanoparticles: The role of ambient ionization in tropospheric aerosol formation, J. Geophy. Res., 106, 4797–4814, 2001.

Yu, F., Luo, G., Bates, T. S., Anderson, B., Clarke, A., Kapustin, V., Yantosca, R. M., Wang, Y., and Wu, S.: Spatial distributions of particle number concentrations in the global troposphere: Simulations, observations, and implications for nucleation mechanisms, J. Geophys. Res., 115, D17205, http://dx.doi.org/10.1029/2009JD013473doi:10.1029/2009JD013473, 2010.

Yung, Y. L. and Demore, W. B.: Photochemistry of the stratosphere of Venus: Implications for atmospheric evolution, Icarus, 51, 199–247, 1982.

Zhang, R., Suh, I., Zhao, J., Zhang, D., Fortner, E. C., Tie, X., Molina, L. T., and Molina, M. J.: Atmospheric new particle formation enhanced by organic acids, Science, 304(5676), 1487–1490, 2004.

Zhao, J. and Turco, R. P.: Nucleation simulations in the wake of a jet aircraft in stratospheric flight, J. Aerosol Sci., 26(5), 779–795, 1995.