Manna, D;
Blumberger, J;
Martin, JML;
Kronik, L;
(2018)
Prediction of electronic couplings for molecular charge transfer using optimally tuned range-separated hybrid functionals.
Molecular Physics
, 116
(19-20)
pp. 2497-2505.
10.1080/00268976.2018.1489084.
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Abstract
Electronic coupling matrix elements are important to the theoretical description of electron transfer processes. However, they are notoriously difficult to obtain accurately from time-dependent density functional theory (TDDFT). Here, we use the HAB11 benchmark dataset of coupling matrix elements to assess whether TDDFT using optimally tuned range-separated hybrid functionals, already known to be successful for the description of charge transfer excitation energies, also allows for an improved accuracy in the prediction of coupling matrix elements. We find that this approach outperforms all previous TDDFT calculations, based on semi-local, hybrid or non-tuned range-separated hybrid functionals, with a remaining average deviation as low as ∼12%. We discuss potential sources for the remaining error.
| Type: | Article |
|---|---|
| Title: | Prediction of electronic couplings for molecular charge transfer using optimally tuned range-separated hybrid functionals |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1080/00268976.2018.1489084 |
| Publisher version: | https://doi.org/10.1080/00268976.2018.1489084 |
| Language: | English |
| Additional information: | This version is the version of record. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | Density functional theory, diabatic states, electronic coupling, range-separated hybrid functionals, optimal tuning |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Physics and Astronomy |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10050770 |
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