Articles | Volume 16, issue 8
Atmos. Chem. Phys., 16, 5299–5313, 2016
Atmos. Chem. Phys., 16, 5299–5313, 2016

Research article 28 Apr 2016

Research article | 28 Apr 2016

The rate of equilibration of viscous aerosol particles

Simon O'Meara1, David O. Topping1,2, and Gordon McFiggans1 Simon O'Meara et al.
  • 1Centre for Atmospheric Science, School of Earth, Atmospheric & Environmental Sciences, University of Manchester, Manchester, M13 9PL, UK
  • 2National Centre for Atmospheric Science (NCAS), University of Manchester, Manchester, M13 9PL, UK

Abstract. The proximity of atmospheric aerosol particles to equilibrium with their surrounding condensable vapours can substantially impact their transformations, fate and impacts and is the subject of vibrant research activity. In this study we first compare equilibration timescales estimated by three different models for diffusion through aerosol particles to assess any sensitivity to choice of model framework. Equilibration times for diffusion coefficients with varying dependencies on composition are compared for the first time. We show that even under large changes in the saturation ratio of a semi-volatile component (es) of 1–90 % predicted equilibration timescales are in agreement, including when diffusion coefficients vary with composition. For condensing water and a diffusion coefficient dependent on composition, a plasticising effect is observed, leading to a decreased estimated equilibration time with increasing final es. Above 60 % final es maximum equilibration times of around 1 s are estimated for comparatively large particles (10 µm) containing a relatively low diffusivity component (1  ×  10−25 m2 s−1 in pure form). This, as well as other results here, questions whether particle-phase diffusion through water-soluble particles can limit hygroscopic growth in the ambient atmosphere. In the second part of this study, we explore sensitivities associated with the use of particle radius measurements to infer diffusion coefficient dependencies on composition using a diffusion model. Given quantified similarities between models used in this study, our results confirm considerations that must be taken into account when designing such experiments. Although quantitative agreement of equilibration timescales between models is found, further work is necessary to determine their suitability for assessing atmospheric impacts, such as their inclusion in polydisperse aerosol simulations.

Short summary
To understand the effect of atmospheric particulate matter on climate and human health we need to know how it evolves. We investigate how best to estimate diffusion of components through particles by comparing diffusion times from three approaches to solving Fick's Law and find that they agree. This means that scientists can simulate Fickian diffusion through atmospheric particles using the approach best suited to their requirements and have confidence that their model is mathematically sound.
Final-revised paper