Uncertainties in quantifying the kinetics of evaporation and condensation of water from atmospheric aerosol are a significant contributor to the uncertainty in predicting cloud droplet number and the indirect effect of aerosols on climate. The influence of aerosol particle surface composition, particularly the impact of surface active organic films, on the condensation and evaporation coefficients remains ambiguous. Here, we report measurements of the influence of organic films on the evaporation and condensation of water from aerosol particles. Significant reductions in the evaporation coefficient are shown to result when condensed films are formed by monolayers of long-chain alcohols [C n H (2n+1) OH], with the value decreasing from 2.4 × 10 −3 to 1.7 × 10 −5 as n increases from 12 to 17. Temperature-dependent measurements confirm that a condensed film of long-range order must be formed to suppress the evaporation coefficient below 0.05. The condensation of water on a droplet coated in a condensed film is shown to be fast, with strong coherence of the long-chain alcohol molecules leading to islanding as the water droplet grows, opening up broad areas of uncoated surface on which water can condense rapidly. We conclude that multicomponent composition of organic films on the surface of atmospheric aerosol particles is likely to preclude the formation of condensed films and that the kinetics of water condensation during the activation of aerosol to form cloud droplets is likely to remain rapid.water transport | organic monolayers | mass accommodation | surface films T he transport of volatile and semivolatile components between the condensed and gas phases in aerosol during evaporation or condensation is important for understanding cloud microphysics, atmospheric chemistry, the delivery of drugs to the lungs, and the applications of aerosols in materials and combustion science. For example, the uptake of chemical species to atmospheric aerosol particles facilitates chemical reactions (1), the condensation of water on cloud condensation nuclei allows cloud droplets to form (2), the uptake of water on pharmaceutical aerosol can affect their deposition pattern within the lungs (3), and the evaporation rates of solvents in spray drying processes influence the structure and morphology of the final microparticle (4). The rate of mass transport to or from an aerosol particle can be considered to involve the interplay of three mechanistic steps: gas phase diffusion, interfacial transfer, and bulk condensed phase diffusion. Different limiting regimes can be identified under which the rate of evaporation or condensation is determined by any one of these steps (5).The Knudsen number is the ratio of the mean free path of gas phase molecules to the particle radius. At low Knudsen number, in the limits of large particle size and high gas pressure, gas phase diffusion usually determines evaporation and condensation rates. Bulk phase diffusion is limiting when the viscosity of the particle impedes transport to or from the surfac...