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Anomalous Behavior of the Homogeneous Ice Nucleation Rate in No-Man's Land

Laksmono, Hartawan (author)
McQueen, Trevor A. (author)
Sellberg, Jonas A. (author)
Stockholms universitet,Fysikum,SLAC National Accelerator Laboratory, USA
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Loh, N. Duane (author)
Huang, Congcong (author)
Schlesinger, Daniel (author)
Stockholms universitet,Fysikum
Sierra, Raymond G. (author)
Hampton, Christina Y. (author)
Nordlund, Dennis (author)
Beye, Martin (author)
Martin, Andrew V. (author)
Barty, Anton (author)
Seibert, M. Marvin (author)
Messerschmidt, Marc (author)
Williams, Garth J. (author)
Boutet, Sebastien (author)
Amann-Winkel, Katrin (author)
Stockholms universitet,Fysikum,University of Innsbruck, Austria
Loerting, Thomas (author)
Pettersson, Lars G. M. (author)
Stockholms universitet,Fysikum
Bogan, Michael J. (author)
Nilsson, Anders (author)
Stockholms universitet,Fysikum,SLAC National Accelerator Laboratory, USA
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 (creator_code:org_t)
2015-07-07
2015
English.
In: Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185 .- 1948-7185. ; 6:14, s. 2826-2832
  • Journal article (peer-reviewed)
Abstract Subject headings
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  • 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 10(3)-10(4) 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 10(6)-10(7) 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.

Subject headings

NATURVETENSKAP  -- Kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences (hsv//eng)
TEKNIK OCH TEKNOLOGIER  -- Nanoteknik (hsv//swe)
ENGINEERING AND TECHNOLOGY  -- Nano-technology (hsv//eng)
NATURVETENSKAP  -- Fysik (hsv//swe)
NATURAL SCIENCES  -- Physical Sciences (hsv//eng)

Keyword

Theoretical Physics
teoretisk fysik

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