Interpretation of the X-Ray Emission Spectra of Liquid Water through Temperature and Isotope Dependence
(2022) In Physical Review Letters 128(8).- Abstract
The interpretation of x-ray emission spectroscopy (XES) spectra in terms of their sensitivity to the hydrogen bonding and the consequent microheterogeneity in liquid water has been debated over a decade. To shed a light on this problem, we report the theoretical reproduction of the debated 1b_{1} peaks observed in the XES spectra of liquid water using semiclassical Kramers-Heisenberg formula. The essence of the temperature and isotope dependence of the 1b_{1} double peaks is explained by molecular dynamics simulations including full vibrational (O─H stretching, bending, and) modes, rotational combined with the density functional theory and core-hole induced dynamics. Some inconsistencies exist with the experimental XES profile, which... (More)
The interpretation of x-ray emission spectroscopy (XES) spectra in terms of their sensitivity to the hydrogen bonding and the consequent microheterogeneity in liquid water has been debated over a decade. To shed a light on this problem, we report the theoretical reproduction of the debated 1b_{1} peaks observed in the XES spectra of liquid water using semiclassical Kramers-Heisenberg formula. The essence of the temperature and isotope dependence of the 1b_{1} double peaks is explained by molecular dynamics simulations including full vibrational (O─H stretching, bending, and) modes, rotational combined with the density functional theory and core-hole induced dynamics. Some inconsistencies exist with the experimental XES profile, which illustrates the need to employ a more precise theoretical calculations for both geometry sampling and electronic structure using a more sophisticated procedure.
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- author
- Takahashi, Osamu ; Yamamura, Ryosuke ; Tokushima, Takashi LU and Harada, Yoshihisa
- organization
- publishing date
- 2022-02-25
- type
- Contribution to journal
- publication status
- published
- subject
- keywords
- Hydrogen Bonding, Isotopes, Temperature, Water/chemistry, X-Rays
- in
- Physical Review Letters
- volume
- 128
- issue
- 8
- article number
- 086002
- publisher
- American Physical Society
- external identifiers
-
- scopus:85125578863
- pmid:35275678
- ISSN
- 1079-7114
- DOI
- 10.1103/PhysRevLett.128.086002
- language
- English
- LU publication?
- yes
- id
- 5efd13af-a095-4a96-8efe-0ede5b5deaaa
- date added to LUP
- 2022-05-12 14:46:17
- date last changed
- 2024-04-21 02:05:18
@article{5efd13af-a095-4a96-8efe-0ede5b5deaaa,
abstract = {{<p>The interpretation of x-ray emission spectroscopy (XES) spectra in terms of their sensitivity to the hydrogen bonding and the consequent microheterogeneity in liquid water has been debated over a decade. To shed a light on this problem, we report the theoretical reproduction of the debated 1b_{1} peaks observed in the XES spectra of liquid water using semiclassical Kramers-Heisenberg formula. The essence of the temperature and isotope dependence of the 1b_{1} double peaks is explained by molecular dynamics simulations including full vibrational (O─H stretching, bending, and) modes, rotational combined with the density functional theory and core-hole induced dynamics. Some inconsistencies exist with the experimental XES profile, which illustrates the need to employ a more precise theoretical calculations for both geometry sampling and electronic structure using a more sophisticated procedure.</p>}},
author = {{Takahashi, Osamu and Yamamura, Ryosuke and Tokushima, Takashi and Harada, Yoshihisa}},
issn = {{1079-7114}},
keywords = {{Hydrogen Bonding; Isotopes; Temperature; Water/chemistry; X-Rays}},
language = {{eng}},
month = {{02}},
number = {{8}},
publisher = {{American Physical Society}},
series = {{Physical Review Letters}},
title = {{Interpretation of the X-Ray Emission Spectra of Liquid Water through Temperature and Isotope Dependence}},
url = {{http://dx.doi.org/10.1103/PhysRevLett.128.086002}},
doi = {{10.1103/PhysRevLett.128.086002}},
volume = {{128}},
year = {{2022}},
}