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Organic aerosol particles play a key role in climate by serving as nucleifor clouds and precipitation. Their sources and composition are highlyvariable, and their phase state ranges from liquid to solid underatmospheric conditions, affecting the pathway of activation to clouddroplets and ice crystals. Due to slow diffusion of water in the particlephase, organic particles may deviate in phase and morphology from theirthermodynamic equilibrium state, hampering the prediction of their influenceon cloud formation. We overcome this problem by combining a novelsemi-empirical method for estimation of water diffusivity with a kineticflux model that explicitly treats water diffusion. We estimate timescalesfor particle deliquescence as well as various ice nucleation pathways for awide variety of organic substances, including secondary organic aerosol(SOA) from the oxidation of isoprene, α-pinene, naphthalene, anddodecane. The simulations show that, in typical atmospheric updrafts, glassystates and solid/liquid core-shell morphologies can persist for long enoughthat heterogeneous ice nucleation in the deposition and immersion mode candominate over homogeneous ice nucleation. Such competition depends stronglyon ambient temperature and relative humidity as well as humidification rateand particle size. Due to differences in glass transition temperature,hygroscopicity and atomic O / C ratio of the different SOA, naphthalene SOA particleshave the highest potential to act as heterogeneous ice nuclei. Our findingsdemonstrate that kinetic limitations of water diffusion into organic aerosolparticles are likely to be encountered under atmospheric conditions and canstrongly affect ice nucleation pathways. For the incorporation of icenucleation by organic aerosol particles into atmospheric models, our resultsdemonstrate a demand for model formalisms that account for the effects ofmolecular diffusion and not only describe ice nucleation onsets as afunction of temperature and relative humidity but also include updraftvelocity, particle size and composition

Competition between water uptake and ice nucleation by glassy organic aerosol particles