Electron-Hole Theory of the Effect of Quantum Nuclei on the X-Ray Absorption Spectra of Liquid Water

被引:41
作者
Sun, Zhaoru [1 ]
Zheng, Lixin [1 ]
Chen, Mohan [1 ]
Klein, Michael L. [1 ,2 ,3 ]
Paesani, Francesco [4 ]
Wu, Xifan [1 ,3 ]
机构
[1] Temple Univ, Dept Phys, Philadelphia, PA 19122 USA
[2] Temple Univ, Dept Chem, Philadelphia, PA 19122 USA
[3] Temple Univ, Inst Computat Mol Sci, Philadelphia, PA 19122 USA
[4] Univ Calif San Diego, Dept Chem & Biochem, Mat Sci & Engn, San Diego Supercomp Ctr, La Jolla, CA 92093 USA
基金
美国国家科学基金会;
关键词
POTENTIAL-ENERGY FUNCTIONS; HYDROGEN-BOND; VIRIAL-COEFFICIENT; SPECTROSCOPY; DYNAMICS; SIMULATIONS; SCATTERING; CLUSTERS; SYSTEMS; SURFACE;
D O I
10.1103/PhysRevLett.121.137401
中图分类号
O4 [物理学];
学科分类号
0702 ;
摘要
Electron-hole excitation theory is used to unveil the role of nuclear quantum effects on the x-ray absorption spectral signatures of water, whose structure is computed via path-integral molecular dynamics with the MB-POL intermolecular potential model. Compared to spectra generated from the classically modeled water, quantum nuclei introduce important effects on the spectra in terms of both the energies and line shapes. Fluctuations due to delocalized protons influence the short-range ordering of the hydrogen bond network via changes in the intramolecular covalence, which broaden the preedge spectra. For intermediate-range and long-range ordering, quantum nuclei approach the neighboring oxygen atoms more closely than classical protons, promoting an "icelike" spectral feature with the intensities shifted from the main edge to the postedge. Computed spectra are in nearly quantitative agreement with the available experimental data.
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页数:6
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