Water diffusion measurements of single charged aerosols using H₂O/D₂O isotope exchange and Raman spectroscopy in an...

Sea spray aerosols contain a large array of organic compounds that contribute to high viscosities at low relative humidity and temperature thereby slowing translational diffusion of water. The Stokes-Einstein equation describes how viscosity is inversely correlated with the translational diffusion coefficient of the diffusing species. However, recent studies indicate that the Stokes-Einstein equation breaks down at high viscosities achieved in the particle phase (>1012 Pa s), underestimating the predicted water diffusion coefficient by orders of magnitude and revealing the need for directly studying the diffusion of water in single aerosols. A new method is reported for measuring the water diffusion coefficient in single suspended charged sucrose-water and citric acid (CA)-water microdroplets in the 30-60 micron diameter range. The translational water diffusion coefficient is quantified using the H2O/D2O isotope exchange technique between 26 and 54% relative humidity (RH) for sucrose and 7 and 25% RH for CA using a recently developed mobile electrodynamic balance apparatus. The results are in good agreement with the literature, particularly the Vignes-type parameterization from experiments using isotope exchange and optical tweezers. Below 15% RH, CA droplets show incomplete H2O/D2O exchange. This mobile electrodynamic balance will allow future studies of atmospherically relevant chemical systems, including field studies.