Intramolecular structure and energetics in supercooled water down to 255 K

被引：16

作者：

Lehmkuehler, Felix ^{[1
,2
]}

Forov, Yury ^{[3
]}

Buening, Thomas ^{[3
]}

Sahle, Christoph J. ^{[4
]}

Steinke, Ingo ^{[1
,2
]}

Julius, Karin ^{[3
]}

Buslaps, Thomas ^{[4
]}

Tolan, Metin ^{[3
]}

Hakala, Mikko ^{[5
]}

Sternemann, Christian ^{[3
]}

机构：

[1] Deutsch Elekt Synchrotron DESY, Notkestr 85, D-22607 Hamburg, Germany

[2] Hamburg Ctr Ultrafast Imaging, Luruper Chaussee 149, D-22761 Hamburg, Germany

[3] Tech Univ Dortmund, DELTA, Fak Phys, D-44221 Dortmund, Germany

[4] European Synchrotron, ESRF, CS 40220, F-38043 Grenoble 9, France

[5] Univ Helsinki, Dept Phys, FI-00014 Helsinki, Finland

来源：

PHYSICAL CHEMISTRY CHEMICAL PHYSICS | 2016年 / 18卷 / 09期

基金：

芬兰科学院;

关键词：

HYDROGEN-BOND NETWORK; LIQUID WATER; RAMAN-SCATTERING; TETRAHYDROFURAN CLATHRATE; TEMPERATURE-DEPENDENCE; HEAT-CAPACITY; EDGE SPECTRUM; ICE; AMBIENT;

D O I：

10.1039/c5cp07721d

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

We studied the structure and energetics of supercooled water by means of X-ray Raman and Compton scattering. Under supercooled conditions down to 255 K, the oxygen K-edge measured by X-ray Raman scattering suggests an increase of tetrahedral order similar to the conventional temperature effect observed in non-supercooled water. Compton profile differences indicate contributions beyond the theoretically predicted temperature effect and provide a deeper insight into local structural changes. These contributions suggest a decrease of the electron mean kinetic energy by 3.3 +/- 0.7 kJ (mol K)(-1) that cannot be modeled within established water models. Our surprising results emphasize the need for water models that capture in detail the intramolecular structural changes and quantum effects to explain this complex liquid.

引用

页码：6925 / 6930

页数：6