2016
DOI: 10.1039/c5cp03919c
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Requirements of first-principles calculations of X-ray absorption spectra of liquid water

Abstract: 1 Abstract A computational benchmark study on X-ray absorption spectra of water has been performed by means of transition-potential density functional theory (TP-DFT), damped time-dependent density functional theory (TDDFT), and damped coupled cluster (CC) linear response theory. For liquid water, using TDDFT with a tailored CAM-B3LYP functional and a polarizable embedding, we find that an embedding with over 2000 water molecules is required to fully converge spectral features for individual molecules, but a s… Show more

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Cited by 43 publications
(98 citation statements)
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“…A similar conclusion for another polarizable embedding QM/MM scheme has been reported in Ref. 66 for converged X-ray absorption spectra averaged over multiple snapshots.…”
Section: E Anionic Pyp Chromophore In Aqueous Solutionsupporting
confidence: 87%
“…A similar conclusion for another polarizable embedding QM/MM scheme has been reported in Ref. 66 for converged X-ray absorption spectra averaged over multiple snapshots.…”
Section: E Anionic Pyp Chromophore In Aqueous Solutionsupporting
confidence: 87%
“…The necessary link between the two properties could be made by accurate calculations of the O K-edge x-ray absorption spectra of H 2 O and D 2 O with particular emphasize of accurately describing the core-excited state potentials at the pre and main edges including the Franck-Condon structure in the core-excited states. Evaluating the at best qualitative agreement of state-of-the art calculations of the O K-edge x-ray absorption spectrum of liquid water with experiment [38][39][40][41][42][43][44][45] shows that there is considerable improvement required in the theoretical descriptions to accurately reproduce and explain the small but significant differences between light and heavy liquid water x-ray absorption spectra.…”
Section: Resultsmentioning
confidence: 99%
“…In order to test the limits of this concept in the x-ray regime it is highly desirable to determine as accurately as possible shift and broadening of the pre-edge peak in the O K-edge absorption spectrum of liquid water. This could further help scrutinizing XAS as a method for probing H-bonded liquids, it could help validating theoretical approaches for calculating the O K-edge absorption spectrum of liquid water [38][39][40][41][42][43][44][45] and it could allow for relating the x-ray spectroscopic observables to the properties of liquid H 2 O and D 2 O by, in particular, potentially enabling to correlate quantum effects, structure and density of states in the liquids.…”
Section: Introductionmentioning
confidence: 99%
“…For these basis sets, the standard regular correlation-consistent basis set is used for hydrogen. In addition, the IGLO-II and IGLO-III basis sets are included since these have been optimised for the calculation of NMR and have been observed previously to perform well for the calculation of core-electron excitations [60,61] as well as the basis sets of Ahlrichs [62] and a triple-zeta quality atomic natural orbital (ANO) basis set [63,64]. Here we only include widely used basis sets that are available for the majority of elements and we do not consider specially designed or modified basis sets, with the exception that the 6-31G(d,p) with uncontracted core basis functions (denoted u6-31G(d,p)) is included.…”
Section: Computational Detailsmentioning
confidence: 99%