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Title: Anomalous behavior of the homogeneous ice nucleation rate in “No-Man’s Land”

Abstract

We present an analysis of ice nucleation kinetics from near-ambient pressure water as temperature decreases below the homogeneous limit T H 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.

Authors:
 [1];  [2];  [3];  [4];  [1];  [5];  [1];  [1];  [1];  [6];  [7];  [7];  [1];  [8];  [1];  [1];  [9];  [10];  [5];  [11] more »;  [3] « less
  1. SLAC National Accelerator Laboratory, Menlo Park, CA (United States)
  2. SLAC National Accelerator Laboratory, Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
  3. SLAC National Accelerator Laboratory, Menlo Park, CA (United States); Stockholm Univ., Stockholm (Sweden)
  4. SLAC National Accelerator Laboratory, Menlo Park, CA (United States); National Univ. of Singapore, (Singapore)
  5. Stockholm Univ., Stockholm (Sweden)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States); Institue for Methods and Instrumentation in Synchrotron Radiation Research, Berlin (Germany)
  7. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  8. SLAC National Accelerator Laboratory, Menlo Park, CA (United States); National Science FOundation BioXFEL Science and Technology Center, Buffalo, NY (United States)
  9. Stockholm Univ., Stockholm (Sweden); Univ. of Innsbruck, Innsbruck (Austria)
  10. Univ. of Innsbruck, Innsbruck (Austria)
  11. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1198682
Alternate Identifier(s):
OSTI ID: 1208831
Grant/Contract Number:  
AC03-76SF00515
Resource Type:
Published Article
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 6; Journal Issue: 14; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; homogeneous ice nucleation; supercooled water; diffusivity; fragile to strong liquid transition; X-ray free-electron laser

Citation Formats

Laksmono, Hartawan, McQueen, Trevor A., Sellberg, Jonas A., Loh, N. Duane, Huang, Congcong, Schlesinger, Daniel, Sierra, Raymond G., Hampton, Christina Y., Nordlund, Dennis, Beye, Martin, Martin, Andrew V., Barty, Anton, Seibert, M. Marvin, Messerschmidt, Marc, Williams, Garth J., Boutet, Sébastien, Amann-Winkel, Katrin, Loerting, Thomas, Pettersson, Lars G. M., Bogan, Michael J., and Nilsson, Anders. Anomalous behavior of the homogeneous ice nucleation rate in “No-Man’s Land”. United States: N. p., 2015. Web. doi:10.1021/acs.jpclett.5b01164.
Laksmono, Hartawan, McQueen, Trevor A., Sellberg, Jonas A., Loh, N. Duane, Huang, Congcong, Schlesinger, Daniel, Sierra, Raymond G., Hampton, Christina Y., Nordlund, Dennis, Beye, Martin, Martin, Andrew V., Barty, Anton, Seibert, M. Marvin, Messerschmidt, Marc, Williams, Garth J., Boutet, Sébastien, Amann-Winkel, Katrin, Loerting, Thomas, Pettersson, Lars G. M., Bogan, Michael J., & Nilsson, Anders. Anomalous behavior of the homogeneous ice nucleation rate in “No-Man’s Land”. United States. doi:10.1021/acs.jpclett.5b01164.
Laksmono, Hartawan, McQueen, Trevor A., Sellberg, Jonas A., Loh, N. Duane, Huang, Congcong, Schlesinger, Daniel, Sierra, Raymond G., Hampton, Christina Y., Nordlund, Dennis, Beye, Martin, Martin, Andrew V., Barty, Anton, Seibert, M. Marvin, Messerschmidt, Marc, Williams, Garth J., Boutet, Sébastien, Amann-Winkel, Katrin, Loerting, Thomas, Pettersson, Lars G. M., Bogan, Michael J., and Nilsson, Anders. Thu . "Anomalous behavior of the homogeneous ice nucleation rate in “No-Man’s Land”". United States. doi:10.1021/acs.jpclett.5b01164.
@article{osti_1198682,
title = {Anomalous behavior of the homogeneous ice nucleation rate in “No-Man’s Land”},
author = {Laksmono, Hartawan and McQueen, Trevor A. and Sellberg, Jonas A. and Loh, N. Duane and Huang, Congcong and Schlesinger, Daniel and Sierra, Raymond G. and Hampton, Christina Y. and Nordlund, Dennis and Beye, Martin and Martin, Andrew V. and Barty, Anton and Seibert, M. Marvin and Messerschmidt, Marc and Williams, Garth J. and Boutet, Sébastien and Amann-Winkel, Katrin and Loerting, Thomas and Pettersson, Lars G. M. and Bogan, Michael J. and Nilsson, Anders},
abstractNote = {We present an analysis of ice nucleation kinetics from near-ambient pressure water as temperature decreases below the homogeneous limit T H 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.},
doi = {10.1021/acs.jpclett.5b01164},
journal = {Journal of Physical Chemistry Letters},
number = 14,
volume = 6,
place = {United States},
year = {2015},
month = {7}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1021/acs.jpclett.5b01164

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Cited by: 34 works
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Works referencing / citing this record:

Evaporating laminar microjets for studies of rapidly evolving structural transformations in supercooled liquids
journal, January 2018