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The role of cluster energy nonaccommodation in atmospheric sulfuric acid nucleation. | LitMetric

The role of cluster energy nonaccommodation in atmospheric sulfuric acid nucleation.

J Chem Phys

Department of Physical Sciences, Division of Atmospheric Sciences, University of Helsinki, P.O. Box 64, Helsinki FIN-00014, Finland.

Published: January 2010

AI Article Synopsis

Article Abstract

We discuss the possible role of energy nonaccommodation (monomer-cluster collisions that do not result in stable product formation due to liberated excess energy) in atmospheric nucleation processes involving sulfuric acid. Qualitative estimates of the role of nonaccommodation are computed using quantum Rice-Ramsberger-Kassel theory together with quantum chemically calculated vibrational frequencies and anharmonic coupling constants for small sulfuric acid-containing clusters. We find that energy nonaccommodation effects may, at most, decrease the net formation rate of sulfuric acid dimers by up to a factor of 10 with respect to the hard-sphere collision rate. A decrease in energy nonaccommodation due to an increasing number of internal degrees of freedom may kinetically slightly favor the participation of amines rather than ammonia as stabilizing agents in sulfuric acid nucleation, though the kinetic enhancement factor is likely to be less than three. However, hydration of the clusters (which always occurs in ambient conditions) is likely to increase the energy accommodation factor, reducing the role that energy nonaccommodation plays in atmospheric nucleation.

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http://dx.doi.org/10.1063/1.3291213DOI Listing

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The role of cluster energy nonaccommodation in atmospheric sulfuric acid nucleation.

J Chem Phys

January 2010

Department of Physical Sciences, Division of Atmospheric Sciences, University of Helsinki, P.O. Box 64, Helsinki FIN-00014, Finland.

We discuss the possible role of energy nonaccommodation (monomer-cluster collisions that do not result in stable product formation due to liberated excess energy) in atmospheric nucleation processes involving sulfuric acid. Qualitative estimates of the role of nonaccommodation are computed using quantum Rice-Ramsberger-Kassel theory together with quantum chemically calculated vibrational frequencies and anharmonic coupling constants for small sulfuric acid-containing clusters. We find that energy nonaccommodation effects may, at most, decrease the net formation rate of sulfuric acid dimers by up to a factor of 10 with respect to the hard-sphere collision rate.

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