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Supercooled water droplets are widely used to study supercooled water [1,2], ice nucleation [3-5], and droplet freezing [6-11]. Their freezing in the atmosphere impacts the dynamics and the climate feedback of clouds [12,13], and can accelerate cloud freezing via secondary ice production [14-17]. Droplet freezing occurs at multiple time and length scales [14,18], 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. Based on 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, while diffraction from the remaining liquid became similar to the one from quasiliquid layers on premelted ice [19,20]. The ice had a strained hexagonal crystal structure just after freezing, which is an early metastable state that likely precedes the formation of ice with stacking defects [8,9,18]. 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.more » « less
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Amaya, Andrew J.; Pathak, Harshad; Modak, Viraj P.; Laksmono, Hartawan; Loh, N. Duane; Sellberg, Jonas A.; Sierra, Raymond G.; McQueen, Trevor A.; Hayes, Matt J.; Williams, Garth J.; et al (, The Journal of Physical Chemistry Letters)
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