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:

Laksmono, Hartawan ^[1]; McQueen, Trevor A. ^[2]; Sellberg, Jonas A. ^[3]; Loh, N. Duane ^[4]; Huang, Congcong ^[5]; Schlesinger, Daniel ^[6]; Sierra, Raymond G. ^[1]; Hampton, Christina Y. ^[1]; Nordlund, Dennis ^[5]; Beye, Martin ^[7]; Martin, Andrew V. ^[8]; Barty, Anton ^[8]; Seibert, M. Marvin ^[9]; Messerschmidt, Marc ^[10]; Williams, Garth J. ^[9]; Boutet, Sébastien ^[9]; Amann-Winkel, Katrin ^[11]; Loerting, Thomas ^[12]; Pettersson, Lars G. M. ^[6]; Bogan, Michael J. ^[1] more »; Nilsson, Anders ^[13] « less

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+ Show Author Affiliations

1. PULSE Institute, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States
2. SUNCAT Ctr Interface Sci & Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States, Department of Chemistry, Stanford University, Stanford, California 94305, United States
3. SUNCAT Ctr Interface Sci & Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States, Department of Physics, AlbaNova University Center, Stockholm University, S-106 91 Stockholm, Sweden
4. PULSE Institute, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States, Center for Bio-Imaging Sciences, National University of Singapore, Singapore 117543
5. Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States
6. Department of Physics, AlbaNova University Center, Stockholm University, S-106 91 Stockholm, Sweden
7. SUNCAT Ctr Interface Sci & Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States, Institute for Methods and Instrumentation in Synchrotron Radiation Research, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Wilhelm-Conrad-Röntgen Campus, Albert-Einstein-Strasse 15, 12489 Berlin, Germany
8. Center for Free-Electron Laser Science, DESY, Notkestrasse 85, 22607 Hamburg, Germany
9. Linac Coherent Light Source, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States
10. Linac Coherent Light Source, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States, National Science Foundation BioXFEL Science and Technology Center, 700 Ellicott Street, Buffalo, New York 14203, United States
11. Department of Physics, AlbaNova University Center, Stockholm University, S-106 91 Stockholm, Sweden, Institute of Physical Chemistry, University of Innsbruck, Innrain 80-82, A-6020 Innsbruck, Austria
12. Institute of Physical Chemistry, University of Innsbruck, Innrain 80-82, A-6020 Innsbruck, Austria
13. SUNCAT Ctr Interface Sci & Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States, Department of Physics, AlbaNova University Center, Stockholm University, S-106 91 Stockholm, Sweden, Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States

Publication Date:

Tue Jul 07 00:00:00 EDT 2015

Research Org.:

SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

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 Name: Journal of Physical Chemistry Letters 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