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Flash Melting Amorphous Ice

Chemical Physics 2023-12-20 v1

Abstract

Water can be vitrified if it is cooled at rates exceeding 31053*10^5 K/s. This makes it possible to outrun crystallization in so-called no man's land, a range of deeply supercooled temperatures where water crystallizes rapidly. One would naively assume that the process can simply be reversed by heating the resulting amorphous ice at a similar rate. We demonstrate that this is not the case. When amorphous ice samples are flash melted with a microsecond laser pulse, time-resolved electron diffraction reveals that the sample transiently crystallizes despite a heating rate of more than 51065*10^6 K/s, demonstrating that the critical heating rate for outrunning crystallization is significantly higher than the critical cooling rate during vitrification. Moreover, we observe different crystallization kinetics for amorphous solid water (ASW) and hyperquenched glassy water (HGW), which suggests that the supercooled liquids formed during laser heating transiently retain distinct non-equilibrium structures that are associated with different nucleation rates. These experiments open up new avenues for elucidating the crystallization mechanism of water and studying its dynamics in no man's land. They also add important mechanistic details to the laser melting and revitrification process that is integral to the emerging field of microsecond time-resolved cryo-electron microscopy.

Keywords

Cite

@article{arxiv.2312.11579,
  title  = {Flash Melting Amorphous Ice},
  author = {Nathan J. Mowry and Constantin R. Krüger and Gabriele Bongiovanni and Marcel Drabbels and Ulrich J. Lorenz},
  journal= {arXiv preprint arXiv:2312.11579},
  year   = {2023}
}

Comments

arXiv admin note: text overlap with arXiv:2211.04419

R2 v1 2026-06-28T13:55:10.932Z