Probing hydrogen bonding orbitals: resonant inelastic soft X-ray scattering of aqueous NH3

被引：46

作者：

Weinhardt, L. ^{[1
,2
,3
,4
]}

Ertan, E. ^{[5
]}

Iannuzzi, M. ^{[6
]}

Weigand, M. ^{[7
]}

Fuchs, O. ^{[7
]}

Baer, M. ^{[8
,9
]}

Blum, M. ^{[2
,10
]}

Denlinger, J. D. ^{[10
]}

Yang, W. ^{[10
]}

Umbach, E. ^{[1
,7
]}

Odelius, M. ^{[5
]}

Heske, C. ^{[1
,2
,3
,4
]}

机构：

[1] Karlsruhe Inst Technol KIT, Inst Photon Sci & Synchrotron Radiat, D-76344 Eggenstein Leopoldshafen, Germany

[2] Univ Nevada, Dept Chem & Biochem, Las Vegas, NV 89154 USA

[3] Karlsruhe Inst Technol, Inst Chem Technol & Polymer Chem, D-76128 Karlsruhe, Germany

[4] Karlsruhe Inst Technol, ANKA Synchrotron Radiat Facil, D-76344 Eggenstein Leopoldshafen, Germany

[5] Stockholm Univ, AlbaNova Univ Ctr, Dept Phys, S-10691 Stockholm, Sweden

[6] Univ Zurich, Inst Chem, CH-8057 Zurich, Switzerland

[7] Univ Wurzburg, Expt Phys 7, D-97074 Wurzburg, Germany

[8] Helmholtz Zentrum Berlin Mat & Energie GmbH, Renewable Energy, D-14109 Berlin, Germany

[9] Brandenburg Tech Univ Cottbus Senftenberg, Inst Phys & Chem, D-03046 Cottbus, Germany

[10] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA

来源：

PHYSICAL CHEMISTRY CHEMICAL PHYSICS | 2015年 / 17卷 / 40期

基金：

瑞典研究理事会;

关键词：

BASIS-SETS; LIQUID WATER; EMISSION SPECTROSCOPY; ELECTRONIC-STRUCTURE; SPECTRA; ABSORPTION; NETWORK; DYNAMICS; SHELL; ATOMS;

D O I：

10.1039/c5cp04898b

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：

To probe the influence of hydrogen bonding on the electronic structure of ammonia, gas phase and aqueous NH3 have been investigated using soft X-ray absorption (XAS), resonant inelastic soft X-ray scattering (RIXS), and electronic structure calculations including dynamical effects. Strong spectral differences in the XAS scans as well as in the RIXS spectra between gas phase and aqueous NH3 are attributed to orbital mixing with the water orbitals, dipole-dipole interactions, differences in vibronic coupling, and nuclear dynamics on the time-scale of the RIXS process. All of these effects are consequences of hydrogen bonding and the impact of the associated orbitals, demonstrating the power of XAS and RIXS as unique tools to study hydrogen bonding in liquids.

引用

页码：27145 / 27153

页数：9

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