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  • Letter
  • Open Access

First-principles quantum Monte Carlo study of charge-carrier mobility in organic molecular semiconductors

Johann Ostmeyer1,*, Tahereh Nematiaram2, Alessandro Troisi3, and Pavel Buividovich1

  • *Contact author: ostmeyer@hiskp.uni-bonn.de
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Phys. Rev. Applied 22, L031004 – Published 10 September, 2024

DOI: https://doi.org/10.1103/PhysRevApplied.22.L031004

Abstract

We present a first-principles numerical study of charge transport in a realistic two-dimensional tight-binding model of organic molecular semiconductors. We use the hybrid Monte Carlo (HMC) algorithm to simulate the full quantum dynamics of phonons and either single or multiple charge carriers without any tunable parameters. We introduce a number of algorithmic improvements, including efficient Metropolis updates for phonon fields based on analytical insights, which lead to negligible autocorrelation times and allow sub-per-mille precisions to be reached at a low computational cost of O(1) CPU hours. Our simulations produce charge-mobility estimates that are in good agreement with experiments and that also justify the phenomenological transient localization approach.

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Phys. Rev. Applied 22, L031004– Published 10 September, 2024
  • Received 5 January 2024
  • Revised 29 May 2024
  • Accepted 13 August 2024
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.

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