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Huisman, Andrew J.
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article
Viscous organic aerosol particles in the upper troposphere
Abstract
New measurements of water diffusion insecondary organic aerosol (SOA) material produced by oxidation ofα-pinene and in a number of organic/inorganic model mixtures(3-methylbutane-1,2,3-tricarboxylic acid (3-MBTCA), levoglucosan,levoglucosan/NH<sub>4</sub>HSO<sub>4</sub>, raffinose) are presented.These indicate that water diffusion coefficients are determined byseveral properties of the aerosol substance and cannot be inferred fromthe glass transition temperature or bouncing properties. Our resultssuggest that water diffusion in SOA particles is faster than oftenassumed and imposes no significant kinetic limitation on water uptakeand release at temperatures above 220 K. The fast diffusion of watersuggests that heterogeneous ice nucleation on a glassy core is veryunlikely in these systems. At temperatures below 220 K, modelsimulations of SOA particles suggest that heterogeneous ice nucleationmay occur in the immersion mode on glassy cores which remain embedded ina liquid shell when experiencing fast updraft velocities. The particlesabsorb significant quantities of water during these updrafts whichplasticize their outer layers such that these layers equilibrate readilywith the gas phase humidity before the homogeneous ice nucleationthreshold is reached. Glass formation is thus unlikely to restricthomogeneous ice nucleation. Only under most extreme conditions near thevery high tropical tropopause may the homogeneous ice nucleation ratecoefficient be reduced as a consequence of slow condensed-phase waterdiffusion. Since the differences between the behavior limited or nonlimited by diffusion are small even at the very high tropicaltropopause, condensed-phase water diffusivity is unlikely to havesignificant consequences on the direct climatic effects of SOA particlesunder tropospheric conditions.