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Modeling Ultrafast Electron Dynamics in Strong Magnetic Fields Using Real-Time Time-Dependent Electronic Structure Methods

Wibowo, Meilani; Irons, Tom J. P.; Teale, Andrew M.

Modeling Ultrafast Electron Dynamics in Strong Magnetic Fields Using Real-Time Time-Dependent Electronic Structure Methods Thumbnail


Authors

ANDREW TEALE Andrew.Teale@nottingham.ac.uk
Professor of Computational and Theoretical Chemistry



Abstract

An implementation of real-time time-dependent Hartree-Fock (RT-TDHF) and current-density-functional theory (RT-TDCDFT) for molecules in strong uniform magnetic fields is presented. In contrast to earlier implementations, the present work enables the use of the RT-TDCDFT formalism, which explicitly includes field dependent terms in the exchange-correlation functional. A range of current dependent exchange-correlation functionals based on the TPSS functional are considered, including a range-separated variant, which is particularly suitable for application to excited state calculations. The performance of a wide range of propagator algorithms for real-time methods is investigated in this context. A recently proposed molecular orbital pair decomposition analysis allows for assignment of electronic transitions, providing detailed information about which molecular orbitals are involved in each excitation. 1 The application of these methods is demonstrated for the electronic absorption spectra of N 2 and H 2 O both in the absence and in the presence of a magnetic field. The dependence of electronic spectra on the magnetic field strength and its orientation relative to the molecule is studied. The complex evolution of the absorption spectra with magnetic field is rationalised using the molecular orbital pair decomposition analysis, which provides crucial insight in strong fields where the spectra are radically different from their zero-field counterparts.

Citation

Wibowo, M., Irons, T. J. P., & Teale, A. M. (2021). Modeling Ultrafast Electron Dynamics in Strong Magnetic Fields Using Real-Time Time-Dependent Electronic Structure Methods. Journal of Chemical Theory and Computation, 17(4), 2137-2165. https://doi.org/10.1021/acs.jctc.0c01269

Journal Article Type Article
Acceptance Date Jan 25, 2021
Online Publication Date Mar 16, 2021
Publication Date Mar 16, 2021
Deposit Date Feb 3, 2021
Publicly Available Date Mar 16, 2021
Journal Journal of Chemical Theory and Computation
Print ISSN 1549-9618
Electronic ISSN 1549-9626
Publisher American Chemical Society
Peer Reviewed Peer Reviewed
Volume 17
Issue 4
Pages 2137-2165
DOI https://doi.org/10.1021/acs.jctc.0c01269
Keywords Physical and Theoretical Chemistry; Computer Science Applications
Public URL https://nottingham-repository.worktribe.com/output/5290760
Publisher URL https://pubs.acs.org/doi/abs/10.1021/acs.jctc.0c01269

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