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How to calculate charge mobility in molecular materials from surface hopping non-adiabatic molecular dynamics – beyond the hopping/band paradigm

Carof, A; Giannini, S; Blumberger, J; (2019) How to calculate charge mobility in molecular materials from surface hopping non-adiabatic molecular dynamics – beyond the hopping/band paradigm. Physical Chemistry Chemical Physics 10.1039/c9cp04770k. (In press). Green open access

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Abstract

Charge transport in high mobility organic semiconductors is in an intermediate regime between small polaron hopping and band transport limits. We have recently shown that surface hopping non-adiabatic molecular dynamics is a powerful method for prediction of charge transport mechanisms in organic materials and for near-quantitative prediction of charge mobilities at room temperature where the effects of nuclear zero-point motion and tunneling are still relatively small [S. Giannini et al., Nat. Commun., 2019, 10, 3843]. Here we assess and critically discuss the extensions to Tully's original method that have led to this success: (i) correction for missing electronic decoherence, (ii) detection of trivial crossings and (iii) removal of decoherence correction-induced spurious charge transfer. If any one of these corrections is not included, the charge mobility diverges with system size, each for different physical reasons. Yet if they are included, convergence with system size, detailed balance and good internal consistency are achieved.

Type: Article
Title: How to calculate charge mobility in molecular materials from surface hopping non-adiabatic molecular dynamics – beyond the hopping/band paradigm
Location: England
Open access status: An open access version is available from UCL Discovery
DOI: 10.1039/c9cp04770k
Publisher version: https://doi.org/10.1039/c9cp04770k
Language: English
Additional information: This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence (http://creativecommons.org/licenses/by-nc/3.0/).
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/10087668
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