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

Ostmeyer, Johann and Nematiaram, Tahereh and Troisi, Alessandro and Buividovich, Pavel (2024) First-principle quantum Monte-Carlo study of charge carrier mobility in organic molecular semiconductors. Physical Review Applied, 22 (3). L031004. ISSN 2331-7043 (https://doi.org/10.1103/PhysRevApplied.22.L031004)

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Abstract

We present a first-principle 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 a 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 analytic insights, which lead to negligible autocorrelation times and allow to reach sub-permille precisions at small computational cost of O(1) CPU-hour. Our simulations produce charge mobility estimates that are in good agreement with experiment and that also justify the phenomenological Transient Localisation approach.

ORCID iDs

Ostmeyer, Johann, Nematiaram, Tahereh ORCID logoORCID: https://orcid.org/0000-0002-0371-4047, Troisi, Alessandro and Buividovich, Pavel;
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