Water Uptake Characteristics of Individual Atmospheric Particles Having Coatings

We used an environmental transmission electron microscope to observe deliquescence and hygroscopic growth of atmospheric particles with hygroscopic coatings over the range 0–100% relative humidity (RH). The particles were collected from polluted and clean environments. Types included a sulfate-coated NaCl/silicate aggregate particle, a sulfate-coated sea-salt particle, and a Mg-rich, chloride-coated sea-salt particle. They all exhibited initial water uptake between 50% and 60% RH, although the first major morphological changes occurred at 70% RH. A deliquescence sphere, adjacent to the core particle, formed between 70% and 76% RH when deliquescence occurred or when the liquid phase was able to break out of the solid exterior coating. The deliquescence sphere grew to engulf the particle with increasing RH. Some particles developed a splatter zone associated with a particle coating. Efflorescence occurred over the range 49–44% RH. Our results indicate that some coated particles undergo a multi-step deliquescence process and that composition of the different phases within the coating affects deliquescence and hygroscopic growth below 76% RH. Above 76% RH, the dominant hygroscopic growth was due to water uptake by NaCl. Efflorescence of these particles also was strongly linked to NaCl, although the presence of other phases inhibited formation of a single NaCl crystal. Our results show that the observed coatings can both enhance particle solubility and lower the effective deliquescence RH of the particle. Thus, these coatings cause important phase and size changes for aerosol particles that could feed back into many other chemical and physical processes that contribute to radiative forcing within the atmosphere