Atmospheric nuclei in the Pacific midtroposphere: Their nature, concentration, and evolution

An extensive flight series was carried out during May-June 1990 in the remote North and South Pacific free troposphere aboard the NASA DC-8. Condensation nuclei counters and optical particle counters provided information on aerosol particles with diameters between 0.003 and 7.0 μm. Vertical profiles revealed aerosol layers to be a common feature of the free troposphere. Regions with highest aerosol mass tended to have the highest concentrations of surface-derived nuclei but the lowest concentrations of total nuclei. Regions with lowest aerosol mass tended to have the highest concentrations of the smaller “ultrafine” condensation nuclei with diameters below 0.02 μm. Horizontal transects totaling over 35,000 km at about 9 to 10-km altitude exhibited variability of approximately 3 orders of magnitude in both aerosol mass and number concentrations over spatial scales ranging from 1 to 1000 km. At these altitudes an approximate inverse relationship between ultrafine concentrations and the surface area of the larger aerosol was evident. Regions having lowest aerosol mass were characterized by aerosol thermal volatility, indicative of a predominately sulfuric acid composition, and by very high concentrations of ultrafine nuclei, indicative of recent homogeneous nucleation. These conditions were frequently observed but were conspicuously evident above cloud over the intertropical convergence zone. The clean, free troposphere appears to be a significant source region for new tropospheric nuclei. A simplified model of the lifetime, coagulation, and cycling of these nuclei suggests that they constitute a source of cloud condensation nuclei in the lower troposphere.

[1]  A. Clarke,et al.  The Pacific marine aerosol: Evidence for natural acid sulfates , 1987 .

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

[3]  A. Clarke A thermo-optic technique for in situ analysis of size-resolved aerosol physicochemistry , 1991 .

[4]  P. Haagenson,et al.  A study of marine aerosols over the Pacific Ocean , 1986 .

[5]  M. H. Smith,et al.  Effect on global warming of wind-dependent aerosol generation at the ocean surface , 1990, Nature.

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

[7]  Vertical Profiles of CCN at Various Geographical Locations , 1973 .

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

[9]  T. Bates,et al.  Regional and seasonal variations in the flux of oceanic dimethylsulfide to the atmosphere , 1987 .

[10]  J. Seinfeld,et al.  Nucleation of sulfuric acid-water and methanesulfonic acid-water solution particles: Implications for the atmospheric chemistry of organosulfur species , 1988 .

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

[12]  J. Katz,et al.  Sulfate aerosol formation and growth in the stratosphere. , 1978, Atmospheric environment.

[13]  B. Barkstrom,et al.  Cloud-Radiative Forcing and Climate: Results from the Earth Radiation Budget Experiment , 1989, Science.

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

[15]  B. Albrecht Aerosols, Cloud Microphysics, and Fractional Cloudiness , 1989, Science.

[16]  C. J. Hahn,et al.  The biogeochemical sulfur cycle in the marine boundary layer over the Northeast Pacific Ocean , 1990 .

[17]  L. Gidel On the maintenance of the marine boundary layer‐free tropospheric gradient of transient tracers , 1983 .

[18]  A. Ono,et al.  Chemical and Physical Properties of Stratospheric Aerosol Particles in the Vicinity of Tropopause Folding , 1989 .

[19]  M. Andreae,et al.  Dimethyl Sulfide in the Surface Ocean and the Marine Atmosphere: A Global View , 1983, Science.

[20]  G. M. Frick,et al.  Submicron aerosol size distributions measured over the tropical and South Pacific , 1990 .

[21]  R. Charlson,et al.  Radiative Properties of the Background Aerosol: Absorption Component of Extinction , 1985, Science.

[22]  John N. Porter,et al.  Aerosol size distribution, composition, and CO2 backscatter at Mauna Loa Observatory , 1991 .

[23]  T. Bates,et al.  Oceanic dimethylsulfide and marine aerosol: Difficulties associated with assessing their covariance , 1989 .

[24]  J. Aítken,et al.  XVI.—The Sun as a Fog Producer. , 1913 .

[25]  J. Seinfeld,et al.  The effects of dimethylsulfide upon marine aerosol concentrations , 1991 .

[26]  R. W. Gillett,et al.  Coherence between seasonal cycles of dimethyl sulphide, methanesulphonate and sulphate in marine air , 1991, Nature.

[27]  P. Crutzen,et al.  Sulfur dioxide in remote oceanic air: Cloud transport of reactive precursors , 1984 .

[28]  C. O'Dowd,et al.  Volatility of aerosol at Mace Head, on the west coast of Ireland , 1990 .

[29]  J. Coakley,et al.  Climate Forcing by Anthropogenic Aerosols , 1992, Science.

[30]  J. Lelieveld,et al.  Zonal average cloud characteristics for global atmospheric chemistry modeling , 1989 .

[31]  E. Bigg,et al.  Origin of Aitken particles in remote regions of the Southern Hemisphere , 1984 .

[32]  John H. Seinfeld,et al.  Simulation of multicomponent aerosol dynamics , 1992 .

[33]  R. Charlson,et al.  Bistability of CCN concentrations and thermodynamics in the cloud-topped boundary layer , 1990, Nature.

[34]  J. Hudson Cloud condensation nuclei near marine cumulus , 1993 .

[35]  H. Akimoto,et al.  Yield of SO2 and formation of aerosol in the photo-oxidation of DMS under atmospheric conditions , 1985 .

[36]  S. Avery,et al.  A trans-Pacific network of wind-profiling Doppler radars for tropical atmospheric research , 1990 .

[37]  S. Schwartz Are global cloud albedo and climate controlled by marine phytoplankton? , 1988, Nature.

[38]  G. Shaw Production of condensation nuclei in clean air by nucleation of H2SO4 , 1989 .

[39]  H. B. Howell,et al.  On the Source and Composition of Cloud Nuclei in a Subsident Air Mass over the North Atlantic , 1970 .

[40]  A. Hogan,et al.  The background level of the summer tropospheric aerosol, sulphur dioxide and ozone over Greenland and the North Atlantic Ocean , 1976 .

[41]  A. Clarke,et al.  Aircraft studies of size‐dependent aerosol sampling through inlets , 1992 .

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

[43]  Methanesulfonic acid and non-sea-salt sulfate in pacific air: Regional and seasonal variations , 1986 .

[44]  THE SUN AS A FOG PRODUCER , 1913 .

[45]  E. Bigg,et al.  Sources of atmospheric particles over Australia , 1978 .