Anomalous Behavior of the Homogeneous Ice Nucleation Rate in No-Man's Land
Number of Authors: 21
2015 (English)In: Journal of Physical Chemistry Letters, ISSN 1948-7185, E-ISSN 1948-7185, Vol. 6, no 14, 2826-2832 p.Article in journal (Refereed) Published
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.
Place, publisher, year, edition, pages
2015. Vol. 6, no 14, 2826-2832 p.
Chemical Sciences Nano Technology Physical Sciences
Research subject Theoretical Physics
IdentifiersURN: urn:nbn:se:su:diva-119545DOI: 10.1021/acs.jpclett.5b01164ISI: 000358339600028OAI: oai:DiVA.org:su-119545DiVA: diva2:847430