Microstructure and crystal order during freezing of supercooled water drops

Armin Kalita, Maximillian Mrozek-McCourt, Thomas F. Kaldawi, Philip R. Willmott, N. Duane Loh, Sebastian Marte, Raymond G. Sierra, Hartawan Laksmono, Jason E. Koglin, Matt J. Hayes, Robert H. Paul, Serge A. H. Guillet, Andrew L. Aquila, Mengning Liang, Sébastien Boutet and Claudiu A. Stan ()
Additional contact information
Armin Kalita: Rutgers University–Newark
Maximillian Mrozek-McCourt: Rutgers University–Newark
Thomas F. Kaldawi: Rutgers University–Newark
Philip R. Willmott: SLAC National Accelerator Laboratory
N. Duane Loh: SLAC National Accelerator Laboratory
Sebastian Marte: Rutgers University–Newark
Raymond G. Sierra: SLAC National Accelerator Laboratory
Hartawan Laksmono: SLAC National Accelerator Laboratory
Jason E. Koglin: SLAC National Accelerator Laboratory
Matt J. Hayes: SLAC National Accelerator Laboratory
Robert H. Paul: SLAC National Accelerator Laboratory
Serge A. H. Guillet: SLAC National Accelerator Laboratory
Andrew L. Aquila: SLAC National Accelerator Laboratory
Mengning Liang: SLAC National Accelerator Laboratory
Sébastien Boutet: SLAC National Accelerator Laboratory
Claudiu A. Stan: Rutgers University–Newark

Nature, 2023, vol. 620, issue 7974, 557-561

Abstract: Abstract Supercooled water droplets are widely used to study supercooled water1,2, ice nucleation3–5 and droplet freezing6–11. Their freezing in the atmosphere affects the dynamics and climate feedback of clouds12,13 and can accelerate cloud freezing through secondary ice production14–17. Droplet freezing occurs at several timescales and length scales14,18 and is sufficiently stochastic to make it unlikely that two frozen drops are identical. Here we use optical microscopy and X-ray laser diffraction to investigate the freezing of tens of thousands of water microdrops in vacuum after homogeneous ice nucleation around 234–235 K. On the basis of drop images, we developed a seven-stage model of freezing and used it to time the diffraction data. Diffraction from ice crystals showed that long-range crystalline order formed in less than 1 ms after freezing, whereas diffraction from the remaining liquid became similar to that from quasi-liquid layers on premelted ice19,20. The ice had a strained hexagonal crystal structure just after freezing, which is an early metastable state that probably precedes the formation of ice with stacking defects8,9,18. The techniques reported here could help determine the dynamics of freezing in other conditions, such as drop freezing in clouds, or help understand rapid solidification in other materials.

Date: 2023
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DOI: 10.1038/s41586-023-06283-2

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