Structural relaxation in supercooled water by time-resolved spectroscopy.

Abstract:

:Water has many kinetic and thermodynamic properties that exhibit an anomalous dependence on temperature, in particular in the supercooled phase. These anomalies have long been interpreted in terms of underlying structural causes, and their experimental characterization points to the existence of a singularity at a temperature of about 225 K. Further insights into the nature and origin of this singularity might be gained by completely characterizing the structural relaxation in supercooled water. But until now, such a characterization has only been realized in simulations that agree with the predictions of simple mode-coupling theory; unambiguous experimental support for this surprising conclusion is, however, not yet available. Here we report time-resolved optical Kerr effect measurements that unambiguously demonstrate that the structural relaxation of liquid and weakly supercooled water follows the behaviour predicted by simple mode-coupling theory. Our findings thus support the interpretation of the singularity as a purely dynamical transition. That is, the anomalous behaviour of weakly supercooled water can be explained using a fully dynamic model and without needing to invoke a thermodynamic origin. In this regard, water behaves like many other, normal molecular liquids that are fragile glass-formers.

journal_name

Nature

journal_title

Nature

authors

Torre R,Bartolini P,Righini R

doi

10.1038/nature02409

keywords:

subject

Has Abstract

pub_date

2004-03-18 00:00:00

pages

296-9

issue

6980

eissn

0028-0836

issn

1476-4687

pii

nature02409

journal_volume

428

pub_type

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