Atmospheric new particle formation: real and apparent growth of neutral and charged particles

Abstract. In this study we have provided simple analytical formulae to estimate the growth rate of a nucleation mode due to self-coagulation and the apparent growth rate due to coagulation scavenging by larger particles. These formulae were used on a set of simulations covering a wide range of atmospheric conditions. The modal growth rates were determined from the simulation results by summing the contribution of each process, by calculating the increase rate in the count mean diameter of the mode and by following the peak concentration of the mode. The results of these three methods were compared with each other and the means used to estimate the growth rate due to self-coagulation and coagulation scavenging were found to give accurate values. We also investigated the role of charged particles and electric interactions in the growth of a nucleation mode. Charged particles were found to increase the growth rate due to both self-coagulation and coagulation scavenging by a factor of ~1.5 to 2. In case of increased condensation onto charged particles, the total condensational growth rate of a nucleation mode may increase significantly in the very early steps of the growth. The analytical formulae provided by this paper were designed to provide the growth rates due to different processes from aerosol dynamic simulations, but the same principles can be used to determine the growth rates from measurement data.

[1]  M. Kulmala,et al.  Variation and balance of positive air ion concentrations in a boreal forest , 2008 .

[2]  Renyi Zhang,et al.  Atmospheric nanoparticles formed from heterogeneous reactions of organics , 2010 .

[3]  Michael R. Zachariah,et al.  Self-Preserving Theory for the Volume Distribution of Particles Undergoing Brownian Coagulation , 2001 .

[4]  M. Kulmala,et al.  On the formation and growth of atmospheric nanoparticles , 2008 .

[5]  J. Smith,et al.  Growth rates of freshly nucleated atmospheric particles in Atlanta , 2005 .

[6]  R. Forkel,et al.  Observations of particle formation and growth in a mountainous forest region in central Europe , 2004 .

[7]  H. Kalesse,et al.  Competition of coagulation sink and source rate: New particle formation in the Pearl River Delta of China , 2010 .

[8]  I. Riipinen,et al.  Initial steps of aerosol growth , 2004 .

[9]  Pasi Aalto,et al.  Atmospheric Chemistry and Physics Discussions , 2001 .

[10]  I. Riipinen,et al.  Aerosol size distribution measurements at four Nordic field stations: identification, analysis and trajectory analysis of new particle formation bursts , 2007 .

[11]  K. Lehtinen,et al.  A model for particle formation and growth in the atmosphere with molecular resolution in size , 2002 .

[12]  T. Petäjä,et al.  Detecting charging state of ultrafine particles : instrumental development and ambient measurements , 2006 .

[13]  G. Mann,et al.  Contribution of particle formation to global cloud condensation nuclei concentrations , 2008 .

[14]  W. H. Walton.  The Mechanics of Aerosols , 1966 .

[15]  J. M. Mäkelä,et al.  On the formation, growth and composition of nucleation mode particles , 2001 .

[16]  A. Arneth,et al.  EUCAARI ion spectrometer measurements at 12 European sites – analysis of new particle formation events , 2010 .

[17]  K. Lehtinen,et al.  Sub-10 nm particle growth by vapor condensation – effects of vapor molecule size and particle thermal speed , 2010 .

[18]  M. Kulmala,et al.  Annual and size dependent variation of growth rates and ion concentrations in boreal forest , 2005 .

[19]  K. Lehtinen,et al.  Effect of condensation rate enhancement factor on 3‐nm (diameter) particle formation in binary ion‐induced and homogeneous nucleation , 2003 .

[20]  P. Roth,et al.  Computer simulation of soot particle coagulation in low pressure flames , 1991 .

[21]  K. Lehtinen,et al.  Charging state of the atmospheric nucleation mode : Implications for separating neutral and ion-induced nucleation , 2007 .

[22]  T. Petäjä,et al.  Factors influencing the contribution of ion-induced nucleation in a boreal forest, Finland , 2009 .

[23]  K. Lehtinen,et al.  Dynamics of atmospheric nucleation mode particles: a timescale analysis , 2004 .

[24]  F. Yu,et al.  Uptake of neutral polar vapor molecules by charged clusters/particles: Enhancement due to dipole‐charge interaction , 2003 .

[25]  T. Bates,et al.  Spatial distributions of particle number concentrations in the global troposphere: Simulations, observations, and implications for nucleation mechanisms , 2010 .

[26]  P. Adams,et al.  Efficiency of cloud condensation nuclei formation from ultrafine particles , 2006 .

[27]  G. Mann,et al.  The contribution of boundary layer nucleation events to total particle concentrations on regional and global scales , 2006 .

[28]  Mark Z. Jacobson,et al.  Fundamentals of Atmospheric Modeling: Preface , 2005 .

[29]  L. Pirjola,et al.  How significantly does coagulational scavenging limit atmospheric particle production , 2001 .

[30]  Pasi Aalto,et al.  Atmospheric Chemistry and Physics on the Growth of Nucleation Mode Particles: Source Rates of Condensable Vapor in Polluted and Clean Environments , 2022 .

[31]  K. Lehtinen,et al.  Ion-UHMA: a model for simulating the dynamics of neutral and charged aerosol particles , 2009 .

[32]  Jack B. Howard,et al.  Coagulation of carbon particles in premixed flames , 1973 .

[33]  G. Mann,et al.  Impact of nucleation on global CCN , 2009 .

[34]  T. Petäjä,et al.  Atmospheric ions and nucleation: a review of observations , 2010 .

[35]  W. Birmili,et al.  The Hohenpeissenberg aerosol formation experiment (HAFEX): a long-term study including size-resolved aerosol, H 2 SO 4 , OH, and monoterpenes measurements , 2002 .

[36]  J. Seinfeld,et al.  Atmospheric Chemistry and Physics: From Air Pollution to Climate Change , 1998 .

[37]  K. Lehtinen,et al.  Estimating nucleation rates from apparent particle formation rates and vice versa: Revised formulation of the Kerminen–Kulmala equation , 2007 .

[38]  G. M. Frick,et al.  Ion—Aerosol Attachment Coefficients and the Steady-State Charge Distribution on Aerosols in a Bipolar Ion Environment , 1986 .

[39]  I. Riipinen,et al.  Toward Direct Measurement of Atmospheric Nucleation , 2007, Science.

[40]  M. Kulmala,et al.  Characterization of new particle formation events at a background site in Southern Sweden: relation to air mass history , 2008 .

[41]  M. Kulmala,et al.  Charging of aerosol particles in the near free-molecule regime , 2004 .

[42]  B. Verheggen,et al.  An inverse modeling procedure to determine particle growth and nucleation rates from measured aerosol size distributions , 2006 .

[43]  Miikka Dal Maso,et al.  Formation and growth of fresh atmospheric aerosols: eight years of aerosol size distribution data from SMEAR II, Hyytiälä, Finland , 2005 .

[44]  C. Kuang,et al.  Determination of cloud condensation nuclei production from measured new particle formation events , 2009 .

[45]  M. Kulmala,et al.  Analysis of one year of Ion-DMPS data from the SMEAR II station, Finland , 2008 .

[46]  K. Lehtinen,et al.  Heterogeneous Nucleation Experiments Bridging the Scale from Molecular Ion Clusters to Nanoparticles , 2008, Science.

[47]  J. Smith,et al.  Estimating nanoparticle growth rates from size-dependent charged fractions: Analysis of new particle formation events in Mexico City , 2008 .

[48]  L. Pirjola,et al.  Stable sulphate clusters as a source of new atmospheric particles , 2000, Nature.

[49]  P. Adams,et al.  Uncertainty in global CCN concentrations from uncertain aerosol nucleation and primary emission rates , 2008 .

[50]  N. Fuchs,et al.  HIGH-DISPERSED AEROSOLS , 1971 .