The violation of the Stokes-Einstein relation in supercooled water

被引:291
作者
Chen, Sow-Hsin
Mallamace, Francesco
Mou, Chung-Yuan
Broccio, Matteo
Corsaro, Carmelo
Faraone, Antonio
Liu, Li
机构
[1] MIT, Dept Nucl Sci & Engn, Cambridge, MA 02139 USA
[2] Univ Messina, Dipartimento Fis, I-98166 Messina, Italy
[3] Univ Messina, Consorzio Nazl Interuniv Sci Fis Mat, I-98166 Messina, Italy
[4] Natl Taiwan Univ, Dept Chem, Taipei 106, Taiwan
关键词
decoupling of transport properties; dynamic crossover; MCM-41;
D O I
10.1073/pnas.0603253103
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
By confining water in nanopores, so narrow that the liquid cannot freeze, it is possible to explore its properties well below its homogeneous nucleation temperature T-H approximate to 235 K. In particular, the dynamical parameters of water can be measured down to 180 K, approaching the suggested glass transition temperature T-g approximate to 165 K. Here we present experimental evidence, obtained from Nuclear Magnetic Resonance and Quasi-Elastic Neutron Scattering spectroscopies, of a well defined decoupling of transport properties (the self-diffusion coefficient and the average translational relaxation time), which implies the breakdown of the Stokes-Einstein relation. We further show that such a non-monotonic decoupling reflects the characteristics of the recently observed dynamic crossover, at approximate to 225 K, between the two dynamical behaviors known as fragile and strong, which is a consequence of a change in the hydrogen bond structure of liquid water.
引用
收藏
页码:12974 / 12978
页数:5
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