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

作者：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 Sebastien; Arnann Winkel Katrin; Loerting Thomas; Pettersson Lars G M; Bogan Michael J; Nilsson Anders^*

来源：Journal of Physical Chemistry Letters, 2015, 6(14): 2826-2832.

DOI：10.1021/acs.jpclett.5b01164

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.

• 出版日期2015-7-16
• 单位国家自然科学基金委员会