Transient spectroscopy from time-dependent electronic-structure theory without multipole expansions
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arXiv
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| Autores principales: | , , , , , , , |
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| Formato: | Preprint |
| Publicado: |
2023
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| _version_ | 1866916359637565440 |
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| author | Aurbakken, Einar Ofstad, Benedicte Sverdrup Kristiansen, Håkon Emil Schøyen, Øyvind Sigmundson Kvaal, Simen Sørensen, Lasse Kragh Lindh, Roland Pedersen, Thomas Bondo |
| author_facet | Aurbakken, Einar Ofstad, Benedicte Sverdrup Kristiansen, Håkon Emil Schøyen, Øyvind Sigmundson Kvaal, Simen Sørensen, Lasse Kragh Lindh, Roland Pedersen, Thomas Bondo |
| contents | Based on the work done by an electromagnetic field on an atomic or molecular electronic system, a general gauge invariant formulation of transient absorption spectroscopy is presented within the semi-classical approximation. Avoiding multipole expansions, a computationally viable expression for the spectral response function is derived from the minimal-coupling Hamiltonian of an electronic system interacting with one or more laser pulses described by a source-free, enveloped electromagnetic vector potential. With a fixed-basis expansion of the electronic wave function, the computational cost of simulations of laser-driven electron dynamics beyond the dipole approximation is the same as simulations adopting the dipole approximation. We illustrate the theory by time-dependent configuration interaction and coupled-cluster simulations of core-level absorption and circular dichroism spectra. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2307_02519 |
| institution | arXiv |
| publishDate | 2023 |
| record_format | arxiv |
| spellingShingle | Transient spectroscopy from time-dependent electronic-structure theory without multipole expansions Aurbakken, Einar Ofstad, Benedicte Sverdrup Kristiansen, Håkon Emil Schøyen, Øyvind Sigmundson Kvaal, Simen Sørensen, Lasse Kragh Lindh, Roland Pedersen, Thomas Bondo Chemical Physics Based on the work done by an electromagnetic field on an atomic or molecular electronic system, a general gauge invariant formulation of transient absorption spectroscopy is presented within the semi-classical approximation. Avoiding multipole expansions, a computationally viable expression for the spectral response function is derived from the minimal-coupling Hamiltonian of an electronic system interacting with one or more laser pulses described by a source-free, enveloped electromagnetic vector potential. With a fixed-basis expansion of the electronic wave function, the computational cost of simulations of laser-driven electron dynamics beyond the dipole approximation is the same as simulations adopting the dipole approximation. We illustrate the theory by time-dependent configuration interaction and coupled-cluster simulations of core-level absorption and circular dichroism spectra. |
| title | Transient spectroscopy from time-dependent electronic-structure theory without multipole expansions |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2307.02519 |