Linear-Response Time-Dependent Embedded Mean-Field Theory

Feizhi Ding, Takashi Tsuchiya, Frederick R. Manby, Thomas F. Miller*

*Corresponding author for this work

Research output: Contribution to journalArticle (Academic Journal)peer-review

16 Citations (Scopus)
215 Downloads (Pure)


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 languageEnglish
Pages (from-to)4216-4227
Number of pages12
JournalJournal of Chemical Theory and Computation
Issue number9
Early online date7 Aug 2017
Publication statusPublished - 12 Sep 2017

Fingerprint Dive into the research topics of 'Linear-Response Time-Dependent Embedded Mean-Field Theory'. Together they form a unique fingerprint.

Cite this