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Modelling Electron Transfers Using Quasidiabatic Hartree-Fock States

Accepted version
Peer-reviewed

Type

Article

Change log

Authors

Jensen, Kristopher T 
Benson, Raz L 
Cardamone, Salvatore 
Thom, Alex JW 

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.

Description

Keywords

physics.chem-ph, physics.chem-ph

Journal Title

Journal of Chemical Theory and Computation

Conference Name

Journal ISSN

1549-9626
1549-9626

Volume Title

14

Publisher

American Chemical Society (ACS)
Sponsorship
Royal Society (uf110161)
Magdalene College, Cambridge for project funding for R.L.B. and K.T.J.