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Linear-response time-dependent embedded mean-field theory

Ding, Feizhi and Tsuchiya, Takashi and Manby, Frederick R. and Miller, Thomas F., III (2017) Linear-response time-dependent embedded mean-field theory. Journal of Chemical Theory and Computation, 13 (9). pp. 4216-4227. ISSN 1549-9618. doi:10.1021/acs.jctc.7b00666.

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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.

Item Type:Article
Related URLs:
URLURL TypeDescription Information
Manby, Frederick R.0000-0001-7611-714X
Miller, Thomas F., III0000-0002-1882-5380
Additional Information:© 2017 American Chemical Society. Received: June 27, 2017; Published: August 7, 2017. This material is based upon work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993. T.F.M. and F.D. additionally acknowledge support from the Air Force Office of Scientific Research under Award Number FA9550-17-1-0102, and T.F.M. acknowledges support from a Camille Dreyfus Teacher-Scholar Award. F.R.M. and T.T. acknowledge support from the Engineering and Physical Sciences Research Council (EP/M013111/1).
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Air Force Office of Scientific Research (AFOSR)FA9550-17-1-0102
Camille and Henry Dreyfus FoundationUNSPECIFIED
Engineering and Physical Sciences Research Council (EPSRC)EP/M013111/1
Issue or Number:9
Record Number:CaltechAUTHORS:20170816-075909755
Persistent URL:
Official Citation:Linear-Response Time-Dependent Embedded Mean-Field Theory Feizhi Ding, Takashi Tsuchiya, Frederick R. Manby, and Thomas F. Miller, III Journal of Chemical Theory and Computation 2017 13 (9), 4216-4227 DOI: 10.1021/acs.jctc.7b00666
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:80460
Deposited By: Tony Diaz
Deposited On:16 Aug 2017 16:26
Last Modified:15 Nov 2021 19:36

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