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

被引：104

作者：

Laksmono, Hartawan ^{[1
]}

McQueen, Trevor A. ^{[2
,3
]}

Sellberg, Jonas A. ^{[2
,4
]}

Loh, N. Duane ^{[1
,5
]}

Huang, Congcong ^{[6
]}

Schlesinger, Daniel ^{[4
]}

Sierra, Raymond G. ^{[1
]}

Hampton, Christina Y. ^{[1
]}

Nordlund, Dennis ^{[6
]}

Beye, Martin ^{[2
,7
]}

Martin, Andrew V. ^{[8
]}

Barty, Anton ^{[8
]}

Seibert, M. Marvin ^{[9
]}

Messerschmidt, Marc ^{[9
,10
]}

Williams, Garth J. ^{[9
]}

Boutet, Sebastien ^{[9
]}

Arnann-Winkel, Katrin ^{[4
,11
]}

Loerting, Thomas ^{[11
]}

Pettersson, Lars G. M. ^{[4
]}

Bogan, Michael J. ^{[1
]}

Nilsson, Anders ^{[2
,4
,6
]}

机构：

[1] PULSE Inst, SLAC Nat Accelerator Lab, Menlo Pk, CA 94025 USA

[2] SUNCAT Ctr Interface Sci & Catalysis, SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA

[3] Stanford Univ, Dept Chem, Stanford, CA 94305 USA

[4] Stockholm Univ, Dept Phys, Alballova Univ Ctr, S-10691 Stockholm, Sweden

[5] Natl Univ Singapore, Ctr Bio Imaging Sci, Singapore 117543, Singapore

[6] SLAC Natl Accelerator Lab, Stanford Synchrotron Radiat Lightsource, Menlo Pk, CA 94025 USA

[7] Helmholtz Zent Berlin Mat & Energie GmbH, Inst Methods & Instrumentat Synchrotron Radiat Re, D-12489 Berlin, Germany

[8] DESY, Ctr Free Electron Laser Sci, D-22607 Hamburg, Germany

[9] SLAC Natl Accelerator Lab, Linac Coherent Light Source, Menlo Pk, CA 94025 USA

[10] Nat Sci Fdn BioXFEL Sci & Technol Ctr, Buffalo, NY 14203 USA

[11] Univ Innsbruck, Inst Phys Chem, A-6020 Innsbruck, Austria

来源：

JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2015年 / 6卷 / 14期

基金：

瑞典研究理事会; 奥地利科学基金会; 美国国家科学基金会;

关键词：

SUPERCOOLED WATER; HYPERQUENCHED WATER; LIQUID TRANSITION; SELF-DIFFUSION; 150; K; CRYSTALLIZATION; DROPLETS; DYNAMICS; KINETICS; TEMPERATURE;

D O I：

10.1021/acs.jpclett.5b01164

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

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.

引用

页码：2826 / 2832

页数：7

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