The homogeneous ice nucleation rate of water droplets produced in a microfluidic device and the role of temperature uncertainty

Abstract

Ice nucleation was investigated experimentally in water droplets with diameters between 53 and 96 micrometres. The droplets were produced in a microfluidic device in which a flow of methyl-cyclohexane and water was combined at the T-junction of micro-channels yielding inverse (water-in-oil) emulsions consisting of water droplets with small standard deviations. In cryo-microscopic experiments we confirmed that upon cooling of such emulsion samples ice nucleation in individual droplets occurred independently of each other as required for the investigation of a stochastic process. The emulsion samples were then subjected to cooling at 1 Kelvin per minute in a differential scanning calorimeter with high temperature accuracy. From the latent heat released by freezing water droplets we inferred the volume-dependent homogeneous ice nucleation rate coefficient of water at temperatures between 236.5 and 237.9 Kelvin. A comparison of our newly derived values to existing rate coefficients from other studies suggests that the volume-dependent ice nucleation rate in supercooled water is slightly lower than previously thought. Moreover, a comprehensive error analysis suggests that absolute temperature accuracy is the single most important experimental parameter determining the uncertainty of the derived ice nucleation rates in our experiments, and presumably also in many previous experiments. Our analysis, thus, also provides a route for improving the accuracy of future ice nucleation rate measurements.