Atmospheric models generally assume that aerosol particles are in equilibrium with the surrounding gas phase. However, recent observations that secondary organic aerosols can exist in a glassy state have highlighted the need to more fully understand the kinetic limitations that may control water partitioning in ambient particles. Here, we explore the influence of slow water diffusion in the condensed aerosol phase on the rates of both condensation and evaporation, demonstrating that significant inhibition in mass transfer occurs for ultraviscous aerosol, not just for glassy aerosol. Using coarse mode (3-4 um radius) ternary sucrose/sodium chloride/aqueous droplets as a proxy for multicomponent ambient aerosol, we demonstrate that the timescale for particle equilibration correlates with bulk viscosity and can be ≫10 3 s. Extrapolation of these timescales to particle sizes in the accumulation mode (e.g., approximately 100 nm) by applying the Stokes-Einstein equation suggests that the kinetic limitations imposed on mass transfer of water by slow bulk phase diffusion must be more fully investigated for atmospheric aerosol. Measurements have been made on particles covering a range in dynamic viscosity from <0.1 to >10 13 Pa s. We also retrieve the radial inhomogeneities apparent in particle composition during condensation and evaporation and contrast the dynamics of slow dissolution of a viscous core into a labile shell during condensation with the slow percolation of water during evaporation through a more homogeneous viscous particle bulk.water uptake | whispering gallery modes | Raman spectroscopy | optical tweezers | viscous aerosol A tmospheric aerosol particles are typically complex mixtures of organic and inorganic species with correspondingly complex equilibria and temporal responses to changes in humidity. Secondary organic aerosols (SOA) continue to receive a great deal of attention due to their impact on radiative forcing, mainly through the indirect effect (1). Ambient aerosol typically contains a significant organic fraction, arising from the oxidation of volatile organic compounds (2). SOA has been largely thought of as existing as a liquid phase, or as a combination of a solid phase within a liquid droplet, but the reality is likely to be far more nuanced. Recently, Virtanen et al. demonstrated that ambient SOA particles can have similar mechanical properties to crystalline ðNH 4 Þ 2 SO 4 particles at 10-20% RH but exist as amorphous glasses to low relative humidity (RH) rather than forming crystalline phases (3). This picture is consistent with the conclusions of Mikhailov et al. (4) and Zobrist et al. (5), who suggested that the existence of glassy states may have profound consequences for the properties of atmospheric aerosol particles, particularly at low temperatures.The term glassy refers to an amorphous, highly viscous state with a dynamic viscosity (η) of greater than 1 × 10 12 Pa s and the mechanical properties of a solid (6). In thermodynamic terms, a glass is in a nonergodic metastable state...