Modelling Electron Transfers Using Quasidiabatic Hartree-Fock States
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Publication Date
2018-09-11Journal Title
Journal of Chemical Theory and Computation
ISSN
1549-9626
Publisher
American Chemical Society (ACS)
Volume
14
Issue
9
Pages
4629-4639
Type
Article
This Version
AM
Metadata
Show full item recordCitation
Jensen, K. T., Benson, R., Cardamone, S., & Thom, A. (2018). Modelling Electron Transfers Using Quasidiabatic Hartree-Fock States. Journal of Chemical Theory and Computation, 14 (9), 4629-4639. https://doi.org/10.1021/acs.jctc.8b00379
Abstract
Electron transfer processes are ubiquitous in chemistry and of great
importance in many systems of biological and commercial interest. The ab-initio
description of these processes remains a challenge in theoretical chemistry,
partly due to the high scaling of many post-Hartree--Fock computational
methods. This poses a problem for systems of interest that are not easily
investigated experimentally. We show that readily available Hartree--Fock
solutions can be used as a quasidiabatic basis to understand electron transfer
reactions in a Marcus framework. Non-orthogonal configuration interaction
calculations can be used to quantify interactions between the resulting
electronic states, and to investigate the adiabatic electron transfer process.
When applied to a titanium-alizarin complex used as a model of a Gr\"atzel-type
solar cell, this approach yields a correct description of the electron transfer
and provides information about the electronic states involved in the process.
Keywords
physics.chem-ph, physics.chem-ph
Sponsorship
Magdalene College, Cambridge for project funding for R.L.B. and K.T.J.
Funder references
Royal Society (uf110161)
Identifiers
External DOI: https://doi.org/10.1021/acs.jctc.8b00379
This record's URL: https://www.repository.cam.ac.uk/handle/1810/292155
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