Anomalous behavior of the homogeneous ice nucleation rate in "no-man's land"

Hartawan Laksmono, Trevor A. McQueen, Jonas A. Sellberg, N. Duane Loh, Congcong Huang, Daniel Schlesinger, Raymond G. Sierra, Christina Y. Hampton, Dennis Nordlund, Martin Beye, Andrew V. Martin, Anton Barty, M. Marvin Seibert, Marc Messerschmidt, Garth J. Williams, Sébastien Boutet, Katrin Amann-Winkel, Thomas Loerting, Lars G.M. Pettersson, Michael J. BoganAnders Nilsson

Research output: Contribution to journalArticle

63 Scopus citations

Abstract

We present an analysis of ice nucleation kinetics from near-ambient pressure water as temperature decreases below the homogeneous limit TH by cooling micrometer-sized droplets (microdroplets) evaporatively at 103-104 K/s and probing the structure ultrafast using femtosecond pulses from the Linac Coherent Light Source (LCLS) free-electron X-ray laser. Below 232 K, we observed a slower nucleation rate increase with decreasing temperature than anticipated from previous measurements, which we suggest is due to the rapid decrease in water's diffusivity. This is consistent with earlier findings that microdroplets do not crystallize at <227 K, but vitrify at cooling rates of 106-107 K/s. We also hypothesize that the slower increase in the nucleation rate is connected with the proposed "fragile-to-strong" transition anomaly in water.

Original languageEnglish (US)
Pages (from-to)2826-2832
Number of pages7
JournalJournal of Physical Chemistry Letters
Volume6
Issue number14
DOIs
StatePublished - Jul 16 2015

Keywords

  • X-ray free-electron laser
  • diffusivity
  • fragile to strong liquid transition
  • homogeneous ice nucleation
  • supercooled water

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

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    Laksmono, H., McQueen, T. A., Sellberg, J. A., Loh, N. D., Huang, C., Schlesinger, D., Sierra, R. G., Hampton, C. Y., Nordlund, D., Beye, M., Martin, A. V., Barty, A., Seibert, M. M., Messerschmidt, M., Williams, G. J., Boutet, S., Amann-Winkel, K., Loerting, T., Pettersson, L. G. M., ... Nilsson, A. (2015). Anomalous behavior of the homogeneous ice nucleation rate in "no-man's land". Journal of Physical Chemistry Letters, 6(14), 2826-2832. https://doi.org/10.1021/acs.jpclett.5b01164