Modelling Electron Transfers Using Quasidiabatic Hartree-Fock States
Jensen, Kristopher T
Benson, Raz L
Thom, Alex JW
Journal of Chemical Theory and Computation
American Chemical Society (ACS)
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Jensen, K. T., Benson, R. L., Cardamone, S., & Thom, A. J. (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
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.
Magdalene College, Cambridge for project funding for R.L.B. and K.T.J.
Royal Society (uf110161)
External DOI: https://doi.org/10.1021/acs.jctc.8b00379
This record's URL: https://www.repository.cam.ac.uk/handle/1810/292155