2021
DOI: 10.1002/wcms.1527
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Modeling of the spectroscopy of core electrons with density functional theory

Abstract: The availability of X‐ray light sources with increased resolution and intensity has provided a foundation for increasingly sophisticated experimental studies exploiting the spectroscopy of core electrons to probe fundamental chemical, physical, and biological processes. Quantum chemical calculations can play a critical role in the analysis of these experimental measurements. The relatively low computational cost of density functional theory (DFT) and time‐dependent density functional theory (TDDFT) make them a… Show more

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Cited by 100 publications
(113 citation statements)
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References 233 publications
(460 reference statements)
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“…From an experimental viewpoint, our ability to generate X-Ray spectra from organic aerosols will be of interest to the theoretical chemistry community. 44 While, theoretical simulations have reached a level of maturity for valence excitations in aqueous systems, 45 there is enormous interest in developing new methods when it comes to core level spectra. 46 Correlations between X-Ray and vibrational spectroscopy at the theoretical level, using the same models of hydrogen bonding networks observed here, will provide a new way to develop an understanding of electronic structure in aqueous organic aerosols.…”
Section: = −mentioning
confidence: 99%
“…From an experimental viewpoint, our ability to generate X-Ray spectra from organic aerosols will be of interest to the theoretical chemistry community. 44 While, theoretical simulations have reached a level of maturity for valence excitations in aqueous systems, 45 there is enormous interest in developing new methods when it comes to core level spectra. 46 Correlations between X-Ray and vibrational spectroscopy at the theoretical level, using the same models of hydrogen bonding networks observed here, will provide a new way to develop an understanding of electronic structure in aqueous organic aerosols.…”
Section: = −mentioning
confidence: 99%
“…This LR-TDDFT formalism has been adapted for the calculation of core excitation spectra using frozen occupied orbitals, 6,33,[57][58][59] i.e., core/valence separation. We will compare this LR-TDDFT approach to the TKDS approach, for benchmark purposes and to highlight advantages of the latter formalism.…”
Section: Lr-tddftmentioning
confidence: 99%
“…Quantum chemistry is currently witnessing a resurgence of interest in x-ray spectroscopy, [1][2][3][4][5][6][7] catalyzed by the emergence of new technologies including coherent ultrahigh harmonic generation, 8 providing capabilities for ultrafast time resolution at x-ray wavelengths, [9][10][11] even with tabletop laser systems. 12 This technology has enabled x-ray absorption spectroscopy (XAS) and x-ray photoelectron spectroscopy (XPS) studies of solution-phase systems, [13][14][15][16] as well as surface-sensitive ultrafast spectroscopy at extreme ultraviolet (XUV) wavelengths.…”
Section: Introductionmentioning
confidence: 99%
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“…XAS calculations with LR-TDDFT can be rendered tractable by means of an activespace approximation that includes only the core orbitals of interest, along with the full virtual space, such that core-to-valence excitations appear as the lowest states in the spectrum. In many-body theory this approximation is known as "core/valence separation", 1,[30][31][32] whereas in LR-TDDFT it has been called the "restricted excitation window" approach, 6,33 but in either case it amounts to freezing most of the occupied orbitals. For excitations at the K-edge (i.e., those originating from 1s orbitals in the occupied space), this approximation introduces negligible errors of ±0.02 eV, 34 although it is less clear what the errors might be for L-or M-edge excitations.…”
Section: Introductionmentioning
confidence: 99%