Measurements of new particle formation and ultrafine particle growth rates at a clean continental site

Simultaneous measurements of aerosol particles and their expected gas phase precursors were made at Idaho Hill, Colorado, a remote continental site. This study used apparatus and techniques similar to those employed in an earlier study at the Mauna Loa Observatory, Hawaii [Weber et al., 1995]. New particle formation, identified by the presence of ultrafine particles (nominally 3 to 4 nm diameter), was commonly observed in downslope (westerly) air and was correlated with high sulfuric acid (H2SO4) concentrations, low relative humidity and low particle surface area concentrations. The data point to H2SO4 as a principle nucleation precursor species with typical daytime concentrations between 106 and 107 molecules cm−3. Particle production was observed at H2SO4 concentrations that are well below predicted values for binary nucleation of H2O and H2SO4, suggesting that another species participated. Particle growth rates were estimated from the data with two independent approaches and in both cases were ∼5 to 10 times higher than can be explained by condensation of H2SO4 and its associated water. This suggests that species in addition to H2S04 were also making large contributions to ultrafine particle growth. Finally, calculated steady-state H2SO4 concentrations were found to be in good agreement with measured values if the mass accommodation coefficient for H2SO4 on aerosol surfaces was assumed equal to ∼1.

[1]  Rodney J. Weber,et al.  New particle formation at a remote continental site: Assessing the contributions of SO2 and organic precursors , 1997 .

[2]  J. Harder,et al.  Meteorological overview of the 1993 OH Photochemistry Experiment , 1997 .

[3]  G. Mount,et al.  An overview of the Tropospheric OH Photochemistry Experiment, Fritz Peak/Idaho Hill, Colorado, fall 1993 , 1997 .

[4]  P. Mcmurry,et al.  Ultrafine Aerosol Measurement Using a Condensation Nucleus Counter with Pulse Height Analysis , 1996 .

[5]  P. Mcmurry,et al.  Fine particle size distributions at the Mauna Loa Observatory, Hawaii , 1996 .

[6]  P. Quinn,et al.  Physical properties of marine boundary layer aerosol particles of the mid-Pacific in relation to sources and meteorological transport , 1996 .

[7]  P. Mcmurry,et al.  MEASURED ATMOSPHERIC NEW PARTICLE FORMATION RATES: IMPLICATIONS FOR NUCLEATION MECHANISMS , 1996 .

[8]  P. Mcmurry,et al.  Measurement of Expected Nucleation Precursor Species and 3–500-nm Diameter Particles at Mauna Loa Observatory, Hawaii , 1995 .

[9]  F. Raes.  Entrainment of free tropospheric aerosols as a regulating mechanism for cloud condensation nuclei in the remote marine boundary layer , 1995 .

[10]  D. Tanner,et al.  Present OH measurement limits and associated uncertainties , 1995 .

[11]  R. Weber,et al.  Studies of New Particle Formation in the Remote Troposphere. , 1995 .

[12]  P. Hobbs,et al.  Further evidence for particle nucleation in clear air adjacent to marine cumulus clouds , 1994 .

[13]  J. W. Fitzgerald,et al.  Marine boundary layer measurements of new particle formation and the effects nonprecipitating clouds have on aerosol size distribution , 1994 .

[14]  Ruprecht Jaenicke,et al.  Number concentration and size distribution of atmospheric aerosol in Siberia , 1994 .

[15]  J. W. Fitzgerald,et al.  A Cloud Chamber Study of the Effect That Nonprecipitating Water Clouds Have on the Aerosol Size Distribution , 1994 .

[16]  A. Clarke.  Atmospheric nuclei in the Pacific midtroposphere: Their nature, concentration, and evolution , 1993 .

[17]  J. Penner,et al.  Large contribution of organic aerosols to cloud-condensation-nuclei concentrations , 1993, Nature.

[18]  D. Hofmann.  Twenty Years Of Balloon-Borne Tropospheric Aerosol Measurements , 1993 .

[19]  D. Tanner,et al.  Measurement of the gas phase concentration of H2SO4 and methane sulfonic acid and estimates of H2SO4 production and loss in the atmosphere , 1993 .

[20]  R. Dingenen,et al.  Simulations of condensation and cloud condensation nuclei from biogenic SO2 in the remote marine boundary layer , 1992 .

[21]  Robert J. Charlson,et al.  Perturbation of the northern hemisphere radiative balance by backscattering from anthropogenic sulfate aerosols , 1991 .

[22]  L. Radke,et al.  Humidity and Particle Fields Around Some Small Cumulus Clouds. , 1991 .

[23]  Peter H. McMurry,et al.  An Ultrafine Aerosol Condensation Nucleus Counter , 1991 .

[24]  L. Radke,et al.  Particle production associated with marine clouds , 1990 .

[25]  James J. Marti.  Diurnal variation in the undisturbed continental aerosol : results from a measurement program in Arizona , 1990 .

[26]  Benjamin Y. H. Liu,et al.  Particle activation and droplet growth processes in condensation nucleus counter—I. Theoretical background☆ , 1990 .

[27]  A. Jaecker-Voirol,et al.  Heteromolecular nucleation in the sulfuric acid-water system , 1989 .

[28]  Richard C. Flagan,et al.  Scanning Electrical Mobility Spectrometer , 1989 .

[29]  P. Mcmurry,et al.  Nucleation and Growth of Aerosol in Chemically Reacting Systems: A Theoretical Study of the Near-Collision-Controlled Regime , 1989 .

[30]  H. O'neal,et al.  Rate constant of the gas phase reaction of SO3 with H2O , 1988 .

[31]  S. Warren,et al.  Oceanic phytoplankton, atmospheric sulphur, cloud albedo and climate , 1987, Nature.

[32]  J. Gleason,et al.  Kinetics of the gas-phase reaction HOSO/sub 2/ + O/sub 2/. -->. HO/sub 2/ + SO/sub 3/ , 1987 .

[33]  M. Molina,et al.  Chemical kinetics and photochemical data for use in stratospheric modeling , 1985 .

[34]  S. Friedlander,et al.  A general correlation for deposition of suspended particles from turbulent gases to completely rough surfaces , 1985 .

[35]  T. L. Wolfe,et al.  An assessment of the impact of pollution on global cloud albedo , 1984 .

[36]  P. Mcmurry.  New particle formation in the presence of an aerosol: Rates, time scales, and sub-0.01 μm size distributions , 1983 .

[37]  Donald E. Hagen,et al.  Linear inversion method to obtain aerosol size distributions from measurements with a differential mobility analyzer , 1983 .

[38]  J. Gras,et al.  On the vapor pressure of sulfuric acid , 1980 .

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

[40]  A. Hogan.  An experiment illustrating that gas conversion by solar radiation is a major influence in the diurnal variation of Aitken nucleus concentrations , 1968 .

[41]  N. Bradbury,et al.  The diurnal variation of atmospheric condensation‐nuclei , 1938 .