References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-8-1577-2008

New particle formation in the Front Range of the Colorado Rocky Mountains

Boy

¹ ² Karl

² Turnipseed

² Mauldin

R. L.

² Kosciuch

² Greenberg

² Rathbone

² Smith

² Held

² Barsanti

² Wehner

³ Bauer

³ Wiedensohler

³ Bonn

⁴ Kulmala

¹ Guenther

Department of Physical Sciences, P.O. Box 64, 00014 Helsinki, Finland

ACD, NCAR, P.O. Box 3000, 80305 Boulder, Colorado, USA

Leibniz Institute for Tropospheric Research, Permoserstrasse 15, 04318 Leipzig, Germany

Department of Plant Physiology, Estonian University of Life Sciences, Kreutzwaldi 64, 51014 Tartu, Estonia

17 03 2008

8 6 1577 1590

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/8/1577/2008/acp-8-1577-2008.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/8/1577/2008/acp-8-1577-2008.pdf

New particle formation is of interest because of its influence on the properties of aerosol population, and due to the possible contribution of newly formed particles to cloud condensation nuclei. Currently no conclusive evidence exists as to the mechanism or mechanisms of nucleation and subsequent particle growth. However, nucleation rates exhibit a clear dependence on ambient sulphuric acid concentrations and particle growth is often attributed to the condensation of organic vapours. A detailed study of new particle formation in the Front Range of the Colorado Rocky Mountains is presented here. Gas and particle measurement data for 32 days was analyzed to identify event days, possible event days, and non-event days. A detailed analysis of nucleation and growth is provided for four days on which new particle formation was clearly observed. Evidence for the role of sesquiterpenes in new particle formation is presented.

References 1

Birmili, W., Stratmann, F., and Wiedensohler, A.: Design of a DMA-based size spectrometer for a large particle size range and stable operation, J. Aerosol Sci., 30(4), 549–554, 1999.

Birmili, W., Berresheim, H., Plass-Dülmer, C., Elste, T., Gilge, S., Wiedensohler, A., and Uhrner, U.: The Hohenpeissenberg aerosol formation experiment (HAFEX): a long-term study including size-resolved aerosol, H2SO4, OH, and monoterpenes measurements, Atmos. Chem. Phys., 3, 361–376, 2003.

Bonn, B., Schuster, G., and Moortgat, G. K.: Influence of water vapor on the process of new particle formation during monoterpenes ozonolysis, J. Phys. Chem. A, 106(12), 2869–2881, 2002.

Bonn, B. and Moortgat, G. K.: Sesquiterpene ozonolysis: Origin of atmospheric new particle formation, Geophys. Res. Lett., 30, 1585, doi:10.1029/GL0017000, 2003.

Bonn, B., Korhonen, H., Petäjä, T, Boy, M., and Kulmala, M.: Understanding the formation of biogenic secondary organic aerosol from $\alpha $-pinene in smog chamber studies: role of organic peroxy radicals, Atmos. Chem. Phys. Discuss., 7, 3901–3939, 2007.

Boy, M. and Kulmala, M.: Nucleation events in the continental boundary layer: Influence of physical and meteorological parameters, Atmos. Chem. Phys., 2, 1–16, 2002.

Boy, M., Rannik, U., Lehtinen, K. E. J., Tarvainen, V., Hakola, H., and Kulmala, M.: Nucleation events in the continental PBL – long term statistical analyses of aerosol relevant characteristics, J. Geophys. Res., 108(D21), 4667, doi:10.1029/2003JD003838, 2003.

Boy, M., Kulmala, M., Ruuskanen, T. M., Pihlatie, M., Reissell, A., Aalto, P. P., Keronen, P., Dal Maso, M., Hellen, H., Hakola, H., Jansson, R., Hanke, M., and Arnold, F.: Sulphuric acid closure and contribution to nucleation mode particle growth, Atmos. Chem. Phys., 5, 863–878, 2005.

Boy, M., Hellmuth, O., Korhonen, H., Nillson, D., ReVelle, D., Turnipseed, A., Arnold, F., and Kulmala, M.: MALTE – Model to predict new aerosol formation in the lower troposphere, Atmos. Chem. Phys., 6, 4499–4517, 2006.

Brazel, A. and Brazel, P.: Summer diurnal wind patterns at Niwot Ridge, CO, Phys. Geog., 4, 53–61, 1983.

Dal Maso, M., Kulmala, M., Riipinen, I., Wagner, R., Hussein, T., Aalto, P. P., and Lehtinen, K. E. J.: Formation and growth of fresh atmospheric aerosols: eight years of aerosol size distribution datat from SMEAR II, Hyytiälä, Finland, Boreal Environ. Res., 10, 323–336, 2006.

De Gouw, J. A., Goldan, P. D., Warneke, C., Kuster, W. C., Roberts, J. M., Marchewka, M., Bertman, S. B., Pszenny, A. A. P., and Keene, W. C.: Validation of proton transfer reaction – mass spectrometry (PTR-MS) measurements of gas-phase organic compounds in the atmosphere during the New England Air Quality Study (NEAQS) in 2002, J. Geophys. Res., 108(D21), 4682, doi:10.1029/2003JD003863, 2003.

Fielder, V., Dal Maso, M., Boy, M., Aufmhoff, H., Hoffmann, J., Schuck, T., Birmili, W., Hanke, M., Uecker, J., Arnold, F., and Kulmala, M.: The contribution of sulphuric acid to atmospheric particle formation and growth: a comparison between boundary layers in Northern and Central Europe, Atmos. Chem. Phys., 5, 1773–1785, 2005.

Fuchs, N. A. and Sutugin, A. G.: High-dispersed aerosols in Topics in Current Aerosol Research, edited by: Hidy, G. M. and Brock, J. R., Pergamon, Oxford, 2, 1–60, 1971.

Großmann, D: Die Gasphasenozonolyse von Alkenen in Gegenwart von Wasserdampf als Quelle f \" ur Wasserstoffperoxid und organische Peroxide in der Atmosphäre, PhD thesis, Mainz University, Mainz, 1999.

Hansel, A., Jordan, A., Warneke, C., Holzinger, R., and Lindinger, W.: Improved detection limit of the proton-transfer reaction mass spectrometer: On-line monitoring of volatile organic compounds at mixing ratios of a few PPTV, Rapid Commun. Mass Sp., 12(13), 871–875, 1998.

Held, A., Nowak, A., Birmili, W., Wiedensohler, A., Forkel, R., and Klemm, O.: Observations of particle formation and growth in a mountainous forest region in Central Europe, J. Geophys. Res., 109, D23204, doi:10.1029/2004JD005346, 2004.

Huey, L. G., Dunlea, E. J., Lovejoy, E. R., Hanson, D. R., Norton, R. B., Fehsenfeld, F. C., and Howard, C. J.: A chemical ionization mass spectrometer for fast time response measurements of HNO3 in air, J. Geophys. Res., 103(D3), 3355–3360, 1998.

Hussein, T., Dal Maso, M., Petäjä, T., Koponen, I. K., Paatero, P., Aalto, P. P., Hämeri, K., and Kulmala, M.: Evaluation of an automatic algorithm for fitting the particle number size distributions, Boreal Environ. Res., 10, 37–355, 2005

Hyvönen, S., Junninen, H., Laakso, L., Dal Maso, M., Grönholm, T., Bonn, B., Keronen, P., Aalto, P., Hiltunen, V., Pohja, T., Launiainen, S., Hari, P., Mannila, H., and Kulmala, M.: A look at aerosol formation using data mining techniques, Atmos. Chem. Phys., 5, 3345–3356, 2005.

Iinuma, Y., Mueller, C., Berndt, T., Böge, O., Claeys, M., and Hrmann, H.: Evidence for the existence of organosulfates from a-pinene ozonolysis in ambient secondary organic aerosol, Environ. Sci. Technol., 41, 6678–6683, 2007.

Kallberer, M., Sax, M., and Asamburova, V.: Molecular size evolution of oligomers in organic aerosols collected in urban atmospheres and generated in a smog chamber, Environ. Sci. Technol., 40, 5917–5922, 2006.

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.

Kerminen, V.-M. and Kulmala, M.: Analytical formulae connecting the "real" and the "apparent" nucleation rate and the nuclei number concentration for atmospheric nucleation events, J. Aerosol Sci., 33, 609–622, 2002.

Korhonen, H., Lehtinen, K. E. J., and Kulmala, M.: Multicomponent aerosol dynamics model UHMA: model development and validation, Atmos. Chem. Phys., 4, 757–771, 2004.

Kulmala, M., Dal Maso, M., Mäkelä, J. M., Pirjola, L., Väkevä, M., Aalto, P., Miikkulainen, P., Hämeri, K., and O'Dowd, C.: On the formation, growth and composition of nucleation mode particles, Tellus B, 53, 479–490, 2001.

Kulmala, M.,Vehkamäki, H., Petäjä, T., Dal Maso, M., Lauri, A., Kerminen, V.-M., Birmili, W., and McMurry, P. H.: Formation and growth rates of ultrafine atmospheric particles: A review of observations, J. Aerosol Sci., 35, 143–176, 2004.

Kulmala, M., Lehtinen, K. E. J., and Laaksonen, A.: Cluster activation theory as an explanation of the linear dependence between formation rate of 3 nm particles and sulphuric acid concentration, Atmos. Chem. Phys., 6, 787–793, 2006,

Kulmala, M., Riipinen, I., Sipilä, M., Manninen, H. E., Petäjä, T., Junninen, H., Dal Maso, M., Mordas, G., Mirme, A., Vana, M., Hirsikko, A., Laakso, L., Harrison, R. M., Hanson, I., Leung, C., Lehtinen, K. E. J., and Kerminen, V.-M.: Toward direct measurement of atmospheric nucleation, Sciencexpress, 318, 89, doi:10.1126science.1144124, 2007.

Lehtinen, K. E. J. and Kulmala, M.: A model for particle formation and growth in the atmosphere with molecular resolution in size, Atmos. Chem. Phys., 3, 251–257, 2003,

Leibrock, E. and Huey, L. G.: Ion chemistry for the detection of isoprene and other volatile organic compounds in ambient air, Geophys. Res. Lett. 27, 12, 1719–1722, 2000.

Lindinger, W., Jordan, A., and Hansel, A.: Proton-transfer-reaction mass spectroscopy (PTR-MS): on-line monitoring of volatile organic compounds at pptv levels, Chem. Soc. Rev., 27, 347–534, 1998.

Lindinger, W., Fall, R., and Karl, T.: Environmental, food and medical applications of Proton-Trnasfer-Reaction Mass Spectrometry (PTR-MS), in: Advances in Gas-Phase Ion Chemistry, edited by: Adams, N. G., Elsevier Science B V., 1–35, 2001.

McMurry, P. H. and Friedlander, S. K.: New particle formation in the presence of an aerosol, Atmos. Environ., 13, 1635–1651, 1979.

Parrish, D. D., Hahn, C. H., Fahey, D. W., Williams, E. J., Bollinger, M. J., Hubler, G., Buhr, M. P., Murphy, P. C., Trainer, M., Hsie, E. Y., Liu, S. C., and Fehsenfeld, F. C.: Systematic variations in the concentrations of NOx (NO Plus NO2) at Niwot Ridge, Colorado, J. Geophys. Res., 95, 1817–1836, 1990.

Riipinen, I., Sihto, S.-L., Kulmala, M., Arnold, F., Dal Maso, M., Birmili, W., Teinilä, K., Kerminen, V.-M., Laaksonen, A., and Lehtinen, K. E. J.: Connections between atmospheric sulphuric acid and new particle formation during QUEST II-IV campaigns in Heidelberg and Hyytiälä, Atmos. Chem. Phys., 7, 1899–1914, 2007.

Shu, Y. and Atkinson, R.: Rate constants for the gas-phase reactions of O<sub>3</sub> with a series of terpenes and OH radical formation from the O<sub>3</sub> reactions with sesquiterpenes at 2962 K, Int. J. Chem. Kin., 26, 1193–1205, 1994.

Sihto, S.-L., Kulmala, M., Kerminen, V.-M., Dal Maso, M., Petäjä, T., Riipinen, I., Korhonen, H., Arnold, F., Janson, R., Boy, M., Laaksonen, A., and Lehtinen, K. E. J.: Atmospheric sulphuric acid and aerosol formation: implications from atmospheric measurements for nucleation and early growth mechanisms, Atmos. Chem. Phys., 6, 4079–4091, 2006.

Surrat, J. D., Kroll, J. H., Kleindienst, T. E., Edney, E. O., Clayes, M., Sorooshinan, A., Ng, N. L., Offenberg, J. H., Lewandowski, M., Jaoui, M., Flagan, R. C., and Seinfeld, J. H.: Evidence for ogransolufates in secondary organic aerosol, Environ. Sci. Technol., 40, 517–527, 2007.

Turnipseed, A. A., Blanken, P. D., Anderson, D. E., and Monson, R. K.: Energy budget above a subalpine forest in complex terrain, Agr. Forest Meteorol., 110, 177–201, 2002.

Wehner, B., Philippin, S., and Wiedensohler, A.: Design and calibration of a thermodenuder with an improved heating unit to measure the size-dependent volatile fraction of aerosol particles, J. Aerosol. Sci., 33, 1087–1093, 2002.

Wu, Z., Hu, M., Liu, S., Wehner, B., Bauer, S., Maßling, A., Wiedensohler, A., Petäjä, T., Dal Maso, M., and Kulmala, M.: New particle formation in Beijing, China: Statistical analysis of a 1-year data set, J. Geophys. Res., 112, D09209, doi:10.1029/2006JD007406, 2007.