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Abstract
We present a time-dependent (TD) linear-response description of excited electronic states within the framework of embedded mean-field theory (EMFT). TD-EMFT allows for subsystems to be described at different mean-field levels of theory, enabling straightforward treatment of excited states and transition properties. We provide benchmark demonstrations of TD-EMFT for both local and nonlocal excitations in organic molecules, as well as applications to chlorophyll a, solvatochromic shifts of a dye in solution, and sulfur K-edge X-ray absorption spectroscopy (XAS). It is found that mixed-basis implementations of TD-EMFT lead to substantial errors in terms of transition properties; however, as previously found for ground-state EMFT, these errors are largely eliminated with the use of Fock-matrix corrections. These results indicate that TD-EMFT is a promising method for the efficient, multilevel description of excited-state electronic structure and dynamics in complex systems.
Original language | English |
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Pages (from-to) | 4216-4227 |
Number of pages | 12 |
Journal | Journal of Chemical Theory and Computation |
Volume | 13 |
Issue number | 9 |
Early online date | 7 Aug 2017 |
DOIs | |
Publication status | Published - 12 Sept 2017 |
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Dive into the research topics of 'Linear-Response Time-Dependent Embedded Mean-Field Theory'. Together they form a unique fingerprint.Projects
- 1 Finished
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Embedded mean-field theory: chemical simulation in complex environments
Manby, F. R. (Principal Investigator)
1/02/15 → 31/05/18
Project: Research