Combining time-dependent density functional theory and the delta scf approach for accurate core-electron spectra
Author(s)
Annegarn, Marcus
Kahk, Juhan Matthias
Lischner, Johannes
Type
Journal Article
Abstract
Spectroscopies that probe electronic excitations from core levels into unoccupied orbitals, such as X-ray absorption spectroscopy and electron energy loss spectroscopy, are widely used to gain insight into the electronic and chemical structure of materials. To support the interpretation of experimental spectra, we assess the performance of a first-principles approach that combines linear-response time-dependent density (TDDFT) functional theory with the Δ self-consistent field (ΔSCF) approach. In particular, we first use TDDFT to calculate the core-level spectrum and then shift the spectrum such that the lowest excitation energy from TDDFT agrees with that from ΔSCF. We apply this method to several small molecules and find encouraging agreement between calculated and measured spectra.
Date Issued
2022-12-13
Date Acceptance
2022-11-01
Citation
Journal of Chemical Theory and Computation, 2022, 18 (12), pp.7620-7629
ISSN
1549-9618
Publisher
American Chemical Society
Start Page
7620
End Page
7629
Journal / Book Title
Journal of Chemical Theory and Computation
Volume
18
Issue
12
Copyright Statement
Copyright © 2022 The Authors. Published by American Chemical Society. This work is published under a CC BY licence.
License URL
Identifier
https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000886494100001&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=a2bf6146997ec60c407a63945d4e92bb
Subjects
BASIS-SETS
Chemistry
Chemistry, Physical
EXCITED-STATES
FINE-STRUCTURE
MOLECULES
Physical Sciences
Physics
Physics, Atomic, Molecular & Chemical
RAY-ABSORPTION SPECTROSCOPY
Science & Technology
Publication Status
Published
Date Publish Online
2022-11-16