Dynamic crossover in deeply cooled water confined in MCM-41 at 4 kbar and its relation to the liquid-liquid transition hypothesis

Zhe Wang; Peisi Le; Kanae Ito; Juscelino B Leão; Madhusudan Tyagi; Sow-Hsin Chen

doi:10.1063/1.4930855

Dynamic crossover in deeply cooled water confined in MCM-41 at 4 kbar and its relation to the liquid-liquid transition hypothesis

J Chem Phys. 2015 Sep 21;143(11):114508. doi: 10.1063/1.4930855.

Authors

Zhe Wang¹, Peisi Le¹, Kanae Ito¹, Juscelino B Leão², Madhusudan Tyagi², Sow-Hsin Chen¹

Affiliations

¹ Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA.
² National Institute of Standards and Technology Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, Maryland 20899, USA.

PMID: 26395720
DOI: 10.1063/1.4930855

Abstract

With quasi-elastic neutron scattering, we study the single-particle dynamics of the water confined in a hydrophilic silica material, MCM-41, at 4 kbar. A dynamic crossover phenomenon is observed at 219 K. We compare this dynamic crossover with the one observed at ambient pressure and find that (a) above the crossover temperature, the temperature dependence of the characteristic relaxation time at ambient pressure exhibits a more evident super-Arrhenius behavior than that at 4 kbar. Especially, at temperatures below about 230 K, the relaxation time at 4 kbar is even smaller than that at ambient pressure. This feature is different from many other liquids. (b) Below the crossover temperature, the Arrhenius behavior found at ambient pressure has a larger activation energy compared to the one found at 4 kbar. We ascribe the former to the difference between the local structure of the low-density liquid (LDL) phase and that of the high-density liquid (HDL) phase, and the latter to the difference between the strength of the hydrogen bond of the LDL and that of the HDL. Therefore, we conclude that the phenomena observed in this paper are consistent with the LDL-to-HDL liquid-liquid transition hypothesis.