References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-11-5591-2011

Particle concentration and flux dynamics in the atmospheric boundary layer as the indicator of formation mechanism

Lauros

¹ Sogachev

² Smolander

¹ Vuollekoski

¹ Sihto

S.-L.

¹ Mammarella

¹ Laakso

¹ ³ ⁴ Rannik

Ü.

¹ Boy

Department of Physics, University of Helsinki, Finland

Wind Energy Division, Risø National Laboratory for Sustainable Energy, Technical University of Denmark, Roskilde, Denmark

Finnish Meteorological Institute, Helsinki, Finland

School of Physical and Chemical Sciences, North-West University, Potchefstroom, Republic of South Africa

16 06 2011

11 12 5591 5601

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/11/5591/2011/acp-11-5591-2011.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/11/5591/2011/acp-11-5591-2011.pdf

We carried out column model simulations to study particle fluxes and deposition and to evaluate different particle formation mechanisms at a boreal forest site in Finland. We show that kinetic nucleation of sulphuric acid cannot be responsible for new particle formation alone as the simulated vertical profile of particle number concentration does not correspond to observations. Instead organic induced nucleation leads to good agreement confirming the relevance of the aerosol formation mechanism including organic compounds emitted by the biosphere. The simulation of aerosol concentration within the atmospheric boundary layer during nucleation event days shows a highly dynamical picture, where particle formation is coupled with chemistry and turbulent transport. We have demonstrated the suitability of our turbulent mixing scheme in reproducing the most important characteristics of particle dynamics within the boundary layer. Deposition and particle flux simulations show that deposition affects noticeably only the smallest particles in the lowest part of the atmospheric boundary layer.

References 1

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, http://dx.doi.org/10.5194/acp-3-361-2003doi:10.5194/acp-3-361-2003, 2003.

Bonn, B., Boy, M., Kulmala, M., Groth, A., Trawny, K., Borchert, S., and Jacobi, S.: A new parametrization for ambient particle formation over coniferous forests and its potential implications for the future, Atmos. Chem. Phys., 9, 8079–8090, http://dx.doi.org/10.5194/acp-9-8079-2009doi:10.5194/acp-9-8079-2009, 2009.

Boy, M., Petäjä, T., Dal Maso, M., Rannik, Ü., Rinne, J., Aalto, P., Laaksonen, A., Vaattovaara, P., Joutsensaari, J., Hoffmann, T., Warnke, J., Apostolaki, M., Stephanou, E. G., Tsapakis, M., Kouvarakis, A., Pio, C., Carvalho, A., Römpp, A., Moortgat, G., Spirig, C., Guenther, A., Greenberg, J., Ciccioli, P., and Kulmala, M.: Overview of the field measurement campaign in Hyytiälä, August 2001 in the framework of the EU project OSOA, Atmos. Chem. Phys., 4, 657–678, http://dx.doi.org/10.5194/acp-4-657-2004doi:10.5194/acp-4-657-2004, 2004.

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, http://dx.doi.org/10.5194/acp-5-863-2005doi:10.5194/acp-5-863-2005, 2005.

Boy, M., Hellmuth, O., Korhonen, H., Nilsson, E. 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, http://dx.doi.org/10.5194/acp-6-4499-2006doi:10.5194/acp-6-4499-2006, 2006.

Boy, M., Kazil, J., Lovejoy, E., Guenther, A., and Kulmala, M.: Relevance of ion-induced nucleation of sulfuric acid and water in the lower troposphere over the boreal forest at northern latitudes, Atmos. Res., 90, 151–158, http://dx.doi.org/10.1016/j.atmosres.2008.01.002doi:10.1016/j.atmosres.2008.01.002, 2008.

Boy, M., Sogachev, A., Lauros, J., Zhou, L., Guenther, A., and Smolander, S.: SOSA – a new model to simulate the concentrations of organic vapours and sulphuric acid inside the ABL – Part 1: Model description and initial evaluation, Atmos. Chem. Phys., 11, 43–51, http://dx.doi.org/10.5194/acp-11-43-2011doi:10.5194/acp-11-43-2011, 2011.

Damian, V.: The kinetic preprocessor KPP-a software environment for solving chemical kinetics, Computers & Chemical Engineering, 26, 1567–1579, http://dx.doi.org/10.1016/S0098-1354(02)00128-Xdoi:10.1016/S0098-1354(02)00128-X, 2002.

Gagné, S., Laakso, L., Petäjä, T., Kerminen, V.-M., and Kulmala, M.: Analysis of one year of Ion-DMPS data from the SMEAR II station, Finland, Tellus, 60B, 318–329, http://dx.doi.org/10.1111/j.1600-0889.2008.00347.xdoi:10.1111/j.1600-0889.2008.00347.x, 2008.

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, http://dx.doi.org/10.5194/acp-6-3181-2006doi:10.5194/acp-6-3181-2006, 2006.

Grönholm, T., Aalto, P P., Hiltunen, V., Rannik, Ü., Rinne, J., Laakso, L., Hyvönen, S., Vesala, T., and Kulmala, M.: Measurements of aerosol particle dry deposition velocity using the relaxed eddy accumulation technique, Tellus, 59B, 381–386, http://dx.doi.org/10.1111/j.1600-0889.2007.00268.xdoi:10.1111/j.1600-0889.2007.00268.x, 2007.

Hao, L. Q., Yli-Pirilä, P., Tiitta, P., Romakkaniemi, S., Vaattovaara, P., Kajos, M. K., Rinne, J., Heijari, J., Kortelainen, A., Miettinen, P., Kroll, J. H., Holopainen, J. K., Smith, J. N., Joutsensaari, J., Kulmala, M., Worsnop, D. R., and Laaksonen, A.: New particle formation from the oxidation of direct emissions of pine seedlings, Atmos. Chem. Phys., 9, 8121–8137, http://dx.doi.org/10.5194/acp-9-8121-2009doi:10.5194/acp-9-8121-2009, 2009.

Hellmuth, O.: Columnar modelling of nucleation burst evolution in the convective boundary layer – first results from a feasibility study Part I: Modelling approach, Atmos. Chem. Phys., 6, 4175–4214, http://dx.doi.org/10.5194/acp-6-4175-2006doi:10.5194/acp-6-4175-2006, 2006a.

Hellmuth, O.: Columnar modelling of nucleation burst evolution in the convective boundary layer – first results from a feasibility study Part II: Meteorological characterisation, Atmos. Chem. Phys., 6, 4215–4230, http://dx.doi.org/10.5194/acp-6-4215-2006doi:10.5194/acp-6-4215-2006, 2006b.

Hellmuth, O.: Columnar modelling of nucleation burst evolution in the convective boundary layer – first results from a feasibility study Part III: Preliminary results on physicochemical model performance using two "clean air mass" reference scenarios, Atmos. Chem. Phys., 6, 4231–4251, http://dx.doi.org/10.5194/acp-6-4231-2006doi:10.5194/acp-6-4231-2006, 2006c.

Hellmuth, O.: Columnar modelling of nucleation burst evolution in the convective boundary layer – first results from a feasibility study Part IV: A compilation of previous observations for valuation of simulation results from a columnar modelling study, Atmos. Chem. Phys., 6, 4253–4274, http://dx.doi.org/10.5194/acp-6-4253-2006doi:10.5194/acp-6-4253-2006, 2006d.

Hoppel, W., Frick, G., Fitzgerald, J., and Larsson, R.: Marine boundary layer measurements of new particle formation and the effects nonprecipitating clouds have on aerosol size distributions, J. Geophys. Res., 99, 14443–14459, 1994.

Korhonen, H., Lehtinen, K. E. J., and Kulmala, M.: Multicomponent aerosol dynamics model UHMA: model development and validation, Atmos. Chem. Phys., 4, 757–771, http://dx.doi.org/10.5194/acp-4-757-2004doi:10.5194/acp-4-757-2004, 2004.

Kuang, C., McMurry, P., McCormick, A., and Eisele, F.: Dependence of nucleation rates on sulfuric acid vapor concentration in diverse atmospheric locations, J. Geophys. Res., 113, D10209, http://dx.doi.org/10.1029/2007JD009253doi:10.1029/2007JD009253, 2008.

Kulmala, M., Hämeri, K K., Aalto, P., Mäkelä, J., Pirjola, L., Nilsson, E D., Buzorius, G., Rannik, Ü., Dal Maso, M., Seidl, W., Hoffmann, T., Jansson, R., Hansson, H.-C., O'Dowd, C., and Viisanen, Y.: Overview of the international project on biogenic aerosol formation in the boreal forest (BIOFOR), Tellus B, 53, 324–343, 2001.

Kulmala, M., Kerminen, V.-M., Anttila, T., Laaksonen, A., and O'Dowd, C D.: Organic aerosol formation via sulphate cluster activation, J. Geophys. Res., 109, D04205, http://dx.doi.org/10.1029/2003JD003961doi:10.1029/2003JD003961, 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, http://dx.doi.org/10.5194/acp-6-787-2006doi:10.5194/acp-6-787-2006, 2006.

Laakso, L., Anttila, T., Lehtinen, K. E. J., Aalto, P. P., Kulmala, M., Hõrrak, U., Paatero, J., Hanke, M., and Arnold, F.: Kinetic nucleation and ions in boreal forest particle formation events, Atmos. Chem. Phys., 4, 2353–2366, http://dx.doi.org/10.5194/acp-4-2353-2004doi:10.5194/acp-4-2353-2004, 2004.

Laakso, L., Grönholm, T., Kulmala, L., Haapanala, S., Hirsikko, A., Lovejoy, E R., Kazil, J., Kurtén, T., Boy, M., Nilsson, E D., Sogachev, A., Riipinen, I., Stratmann, F., and Kulmala, M.: Hot-air balloon as a platform for boundary layer profile measurements during particle formation, Boreal Environ. Res., 12, 279–294, 2007.

Lauros, J., Nilsson, E. D., Dal Maso, M., and Kulmala, M.: Contribution of mixing in the ABL to new particle formation based on observations, Atmos. Chem. Phys., 7, 4781–4792, http://dx.doi.org/10.5194/acp-7-4781-2007doi:10.5194/acp-7-4781-2007, 2007.

Makkonen, R., Asmi, A., Korhonen, H., Kokkola, H., Järvenoja, S., Räisänen, P., Lehtinen, K. E. J., Laaksonen, A., Kerminen, V.-M., Järvinen, H., Lohmann, U., Bennartz, R., Feichter, J., and Kulmala, M.: Sensitivity of aerosol concentrations and cloud properties to nucleation and secondary organic distribution in ECHAM5-HAM global circulation model, Atmos. Chem. Phys., 9, 1747–1766, http://dx.doi.org/10.5194/acp-9-1747-2009doi:10.5194/acp-9-1747-2009, 2009.

Manninen, H. E., Nieminen, T., Riipinen, I., Yli-Juuti, T., Gagné, S., Asmi, E., Aalto, P. P., Petäjä, T., Kerminen, V.-M., and Kulmala, M.: Charged and total particle formation and growth rates during EUCAARI 2007 campaign in Hyytiälä, Atmos. Chem. Phys., 9, 4077–4089, http://dx.doi.org/10.5194/acp-9-4077-2009doi:10.5194/acp-9-4077-2009, 2009.

McMurry, P. and Friedlander, S.: New particle formation in the presence of an aerosol, Atmos. Environ., 13, 1635–1651, http://dx.doi.org/10.1016/0004-6981(79)90322-6doi:10.1016/0004-6981(79)90322-6, 1979.

Napari, I., Noppel, M., Vehkamäki, H., and Kulmala, M.: An improved model for ternary nucleation of sulfuric acid-ammonia-water, J. Chem. Phys., 116, 4221–4227, 2002.

Noh, Y., Cheon, W G., Hong, S.-Y., and Raasch, S.: Improvement of the K-profile model for the planetary boundary layer based on large eddy simulation data, Bound. Lay. Meteor., 107, 401–427, 2003.

O'Dowd, C. D., Yoon, Y. J., Junkermann, W., Aalto, P., Kulmala, M., Lihavainen, H., and Viisanen, Y.: Airborne measurements of nucleation mode particles II: boreal forest nucleation events, Atmos. Chem. Phys., 9, 937–944, http://dx.doi.org/10.5194/acp-9-937-2009doi:10.5194/acp-9-937-2009, 2009.

Paasonen, P., Nieminen, T., Asmi, E., Manninen, H. E., Petäjä, T., Plass-Dülmer, C., Flentje, H., Birmili, W., Wiedensohler, A., Hõrrak, U., Metzger, A., Hamed, A., Laaksonen, A., Facchini, M. C., Kerminen, V.-M., and Kulmala, M.: On the roles of sulphuric acid and low-volatility organic vapours in the initial steps of atmospheric new particle formation, Atmos. Chem. Phys., 10, 11223–11242, http://dx.doi.org/10.5194/acp-10-11223-2010doi:10.5194/acp-10-11223-2010, 2010.

Petroff, A., Mailliat, A., Amielh, M., and Anselmet, F.: Aerosol dry deposition on vegetative canopies. Part II: A new modelling approach and applications, Atmos. Environ., 42, 3654–3683, http://dx.doi.org/10.1016/j.atmosenv.2007.12.060doi:10.1016/j.atmosenv.2007.12.060, 2008.

Petäjä, T., Mauldin, III, R. L., Kosciuch, E., McGrath, J., Nieminen, T., Paasonen, P., Boy, M., Adamov, A., Kotiaho, T., and Kulmala, M.: Sulfuric acid and OH concentrations in a boreal forest site, Atmos. Chem. Phys., 9, 7435–7448, http://dx.doi.org/10.5194/acp-9-7435-2009doi:10.5194/acp-9-7435-2009, 2009.

Pryor, S., Gallagher, M., Sievering, H., Larsen, S., Barthelmie, R., Birsan, F., Nemitz, E., Rinne, J., Kulmala, M., Grönholm, T., Taipale, R., and Vesala, T.: A review of measurement and modelling results of particle atmosphere–surface exchange, Tellus B, 60, 42–75, http://dx.doi.org/10.1111/j.1600-0889.2007.00298.xdoi:10.1111/j.1600-0889.2007.00298.x, 2008.

Radhakrishnan, K. and Hindmarsh, A C.: Description and Use of LSODE, the Livermore Solver for Ordinary Differential Equations, Tech. Rep. report UCRL-ID-113855, Lawrence Livermore National Laboratory, 1993.

Rannik, Ü., Aalto, P., Keronen, P., Vesala, T., and Kulmala, M.: Interpretation of aerosol particle fluxes over a pine forest: Dry deposition and random errors, J. Geophys. Res., 108, 4544, http://dx.doi.org/10.1029/2003JD003542doi:10.1029/2003JD003542, 2003.

Riipinen, I., Sihto, S.-L., Kulmala, M., Arnold, F., Dal Maso, M., Birmili, W., Saarnio, K., Teinilä, K., Kerminen, V.-M., Laaksonen, A., and Lehtinen, K. E. J.: Connections between atmospheric sulphuric acid and new particle formation during QUEST III–IV campaigns in Heidelberg and Hyytiälä, Atmos. Chem. Phys., 7, 1899–1914, http://dx.doi.org/10.5194/acp-7-1899-2007doi:10.5194/acp-7-1899-2007, 2007.

Sandu, A. and Sander, R.: Technical note: Simulating chemical systems in Fortran90 and Matlab with the Kinetic PreProcessor KPP-2.1, Atmos. Chem. Phys., 6, 187–195, http://dx.doi.org/10.5194/acp-6-187-2006doi:10.5194/acp-6-187-2006, 2006.

Sandu, A., Verwer, J G., Loon, M V., Carmichael, G R., Potra, F A., Dabdub, D., and Seinfeld, J H.: Benchmarking stiff ode solvers for atmospheric chemistry problems-I. implicit vs explicit, Atmos. Environ., 31, 3151–3166, http://dx.doi.org/10.1016/S1352-2310(97)00059-9doi:10.1016/S1352-2310(97)00059-9, 1997.

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, http://dx.doi.org/10.5194/acp-6-4079-2006doi:10.5194/acp-6-4079-2006, 2006.

Sihto, S.-L., Vuollekoski, H., Leppä, J., Riipinen, I., Kerminen, V.-M., Korhonen, H., Lehtinen, K. E. J., Boy, M., and Kulmala, M.: Aerosol dynamics simulations on the connection of sulphuric acid and new particle formation, Atmos. Chem. Phys., 9, 2933–2947, http://dx.doi.org/10.5194/acp-9-2933-2009doi:10.5194/acp-9-2933-2009, 2009.

Sogachev, A.: A note on two-equation closure modelling of canopy flow, Bound. Lay. Meteorol., 130, 423–435, 2009.

Sogachev, A. and Panferov, O.: Modification of two-equation models to account for plant drag, Bound. Lay. Meteorol., 121, 229–266, http://dx.doi.org/10.1007/s10546-006-9073-5doi:10.1007/s10546-006-9073-5, 2006.

Sogachev, A., Menzhulin, G V., Heimann, M., and Lloyd, J.: A simple three-dimensional canopy – planetary boundary layer simulation model for scalar concentrations and fluxes, Tellus, 54B, 784–819, 2002.

Stratmann, F., Siebert, H., Spindler, G., Wehner, B., Althausen, D., Heintzenberg, J., Hellmuth, O., Rinke, R., Schmieder, U., Seidel, C., Tuch, T., Uhrner, U., Wiedensohler, A., Wandinger, U., Wendisch, M., Schell, D., and Stohl, A.: New-particle formation events in a continental boundary layer: first results from the SATURN experiment, Atmos. Chem. Phys., 3, 1445–1459, http://dx.doi.org/10.5194/acp-3-1445-2003doi:10.5194/acp-3-1445-2003, 2003.

Stull, R B.: An Introduction to Boundary Layer Meteorology, Kluwer Academic Publishers, Dordrecht, The Netherlands, 670~p., ISBN: 90-227-2969-4, 1989.

Vehkamäki, H., Kulmala, M., Lehtinen, K., Timmreck, C., Noppel, M., and Laaksonen, A.: An Improved Parameterization for Sulfuric Acid–water Nucleation Rates for Tropospheric and Stratospheric Conditions, J. Geophys. Res., 107, 4622, http://dx.doi.org/10.1029/2002JD002184doi:10.1029/2002JD002184, 2002.

Vuollekoski, H., Nieminen, T., Paasonen, P., Sihto, S.-L., Boy, M., Manninen, H., Lehtinen, K. E J., Kerminen, V.-M., and Kulmala, M.: Atmospheric nucleation and initial steps of particle growth: numerical comparison of different theories and hypotheses, Atmos. Res., 98, 229–236, http://dx.doi.org/10.1016/j.atmosres.2010.04.007doi:10.1016/j.atmosres.2010.04.007, 2010.

Weber, R., Marti, J., McMurry, P., Eisele, F., Tanner, D., and Jefferson, A.: Measured atmospheric new particle formation rates: Implications for nucleation mechanisms, Chem. Eng. Commun., 151, 53–64, 1996.

Weber, R., Marti, J., McMurry, P., Eisele, F., Tanner, D., and Jefferson, A.: Measurements of new particle formation and ultrafine particle growth rates at a clean continental site, J. Geophys. Res., 102, 4375–4385, 1997.