Homogeneous freezing nucleation rates and crystallization dynamics of single levitated sulfuric acid solution droplets

Supercooled sulfuric acid solution droplets are a major constituent of the stratospheric background aerosol. We report the rate of homogeneous freezing and the crystallization dynamics of single levitated sulfuric acid solution droplets with 0 to 57.6 wt.% H2SO4. The energy of formation of the critical nucleus and the self-diffusion activation energy are deduced from the experiments as a function of temperature and concentration. The results are compared to both theoretical and experimental work of other groups.

[1]  B. Berge,et al.  Fast in situ sizing technique for single levitated liquid aerosols. , 1999, Applied optics.

[2]  T. Leisner,et al.  Homogeneous nucleation rates of supercooled water measured in single levitated microdroplets , 1999 .

[3]  A. Bertram,et al.  Mechanisms and Temperatures for the Freezing of Sulfuric Acid Aerosols Measured by FTIR Extinction Spectroscopy , 1996 .

[4]  D. Rogers,et al.  Freezing nucleation rates of dilute solution droplets measured between-30 and-40 C in labo-ratory si , 1990 .

[5]  S. H. Maron,et al.  Phase Equilibria of the System Sulfur Trioxide-Water1 , 1950 .

[6]  G. R. Wood,et al.  Homogeneous Nucleation Kinetics of Ice from Water , 1970 .

[7]  P. Hamill,et al.  Homogeneous freezing nucleation of stratospheric solution droplets , 1991 .

[8]  F. S. Long,et al.  Viscosity of Supercooled Sulfuric Acid Solutions , 1995 .

[9]  H. R. Pruppacher,et al.  A New Look at Homogeneous Ice Nucleation in Supercooled Water Drops , 1995 .

[10]  P. Crutzen,et al.  Freezing of HNO3/H2SO4/H2O Solutions at Stratospheric Temperatures: Nucleation Statistics and Experiments , 1997 .

[11]  A. Prenni,et al.  Crystallization Kinetics of Nitric Acid Dihydrate Aerosols , 1996 .

[12]  M. Molina,et al.  A NEW OPTICAL TECHNIQUE TO STUDY AEROSOL PHASE TRANSITIONS : THE NUCLEATION OF ICE FROM H2SO4 AEROSOLS , 1998 .

[13]  Michael D. Barnes,et al.  A CCD BASED APPROACH TO HIGH-PRECISION SIZE AND REFRACTIVE INDEX DETERMINATION OF LEVITATED MICRODROPLETS USING FRAUNHOFER DIFFRACTION , 1997 .

[14]  R. F. Wuerker,et al.  Electrodynamic Containment of Charged Particles , 1959 .

[15]  D. Imre,et al.  Phase transformations in sulfuric acid aerosols: Implications for stratospheric ozone depletion , 1997 .

[16]  H. Pruppacher Self‐Diffusion Coefficient of Supercooled Water , 1972 .

[17]  N. Larsen The impact of freezing of sulfate aerosols on the formation of polar startospheric clouds , 1994 .

[18]  A. Heymsfield,et al.  Cirrus crystal nucleation by homogeneous freezing of solution droplets , 1989 .