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The End of Ice I

submitted on 10.07.2019, 20:59 and posted on 11.07.2019, 13:18 by Daniel R. Moberg, Daniel Becker, Christoph W. Dierking, Florian Zurheide, Bernhard Bandow, Udo Buck, Arpa Hudait, Valeria Molinero, Paesani Lab, Thomas Zeuch

The appearance of ice I in the smallest possible clusters and the nature of its phase coexistence with liquid water could not thus far be unravelled. The experimental and theoretical infrared spectroscopic and free energy results of this work show the emergence of the characteristic hydrogen bonding pattern of ice I in clusters containing only around 90 water molecules. The onset of crystallization is accompanied by an increase of surface oscillator intensity with decreasing surface to volume ratio, a new spectral indicator of nanoscale crystallinity of water. In the size range from 90 to 150 water molecules, we observe mixtures of largely crystalline and purely amorphous clusters. Our analysis suggests that the liquid-ice I transition in clusters loses its sharp first-order character at the end of the crystalline size regime and occurs over a range of temperatures through heterophasic oscillations in time, a process without analog in bulk water.


National Science Foundation

Deutsche Forschungsgemeinschaft


Email Address of Submitting Author


University of California, San Diego


United States

ORCID For Submitting Author


Declaration of Conflict of Interest

No conflict of interest