ABSTRACT
The mass accommodation coefficient αM of water on aqueous triethylene glycol droplets was determined for water mole fractions in the range xmol = 0.1-0.93 and temperatures between 21 and 26 °C from modulated Mie scattering measurement on single optically-trapped droplets in combination with a kinetic multilayer model. αM reaches minimum values around 0.005 at a critical water concentration of xmol = 0.38, and increases with decreasing water content to a value of ≈0.1 for almost pure triethylene glycol droplets, essentially independent of the temperature. Above xmol = 0.38, αM first increases with increasing water content and then stabilises at a value of ≈0.1 at the lowest temperatures, while at the highest temperature its value remains around 0.005. We analysed the unexpected concentration and temperature dependence with a previously proposed two-step model for mass accommodation which provides concentration and temperature-dependent activation enthalpies and entropies. We suggest that the unexpected minimum in αM at intermediate water concentrations might arise from a more or less saturated hydrogen-bond network that forms at the droplet surface.
ABSTRACT
Sea salt aerosol is among the most abundant aerosol species in Earth's atmosphere, and its hygroscopicity is an important parameter to quantify its interaction with solar radiation. Conflicting values for the hygroscopic growth have been reported in the literature, which decreases the accuracy with which their impact on Earth's climate can be modelled. Here we report new values of the hygroscopic growth for a selection of salt compositions representative of atmospheric sea salt. These values are obtained from single optically trapped aqueous droplets with dry radii between 0.3 and 2 µm, using a recently developed method for single particle mass measurement in an optical trap. We compare our results to earlier studies and propose a way to reconcile the apparent discrepancies found in the literature. Within our studies, we also observe the crystallization of CaSO4·2H2O (Gypsum) during the drying of optically trapped sea salt droplets at significantly larger relative humidity of 65-68% than the main efflorescence relative humidity at 50%. This preceding transition occurred in the absence of any contact of the particle with a surface.
ABSTRACT
The uptake of water vapor by various organic aerosols is important in a number of applications ranging from medical delivery of pharmaceutical aerosols to cloud formation in the atmosphere. The coefficient that describes the probability that the impinging gas-phase molecule sticks to the surface of interest is called the mass accommodation coefficient, αM. Despite the importance of this coefficient for the description of water uptake kinetics, accurate values are still lacking for many systems. In this Feature Article, we present various experimental techniques that have been evoked in the literature to study the interfacial transport of water and discuss the corresponding strengths and limitations. This includes our recently developed technique called photothermal single-particle spectroscopy (PSPS). The PSPS technique allows for a retrieval of αM values from three independent, yet simultaneous measurements operating close to equilibrium, providing a robust assessment of interfacial mass transport. We review the currently available data for αM for water on various organics and discuss the few studies that address the temperature and relative humidity dependence of αM for water on organics. The knowledge of the latter, for example, is crucial to assess the water uptake kinetics of organic aerosols in the Earth's atmosphere. Finally, we argue that PSPS might also be a viable method to better restrict the αM value for water on liquid water.
