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

Johann  Ostmeyer; Tahereh Nematiaram; Alessandro Troisi; Pavel  Buividovich

doi:10.1103/PhysRevApplied.22.L031004

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

Johann Ostmeyer, Tahereh Nematiaram, Alessandro Troisi, Pavel Buividovich

Pure And Applied Chemistry

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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.

Original language	English
Article number	L031004
Number of pages	21
Journal	Physical Review Applied
Volume	22
Issue number	3
DOIs	https://doi.org/10.1103/PhysRevApplied.22.L031004
Publication status	Published - 10 Sept 2024

Funding

This work was funded in part by the STFC Consolidated Grant no. ST/T000988/1 and by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) as part of the CRC 1639 NuMeriQS – project no. 511713970. A.T. thanks the European Research Council (Grant No. 101020369) for supporting his research.

Keywords

organic molecular semiconductors
Hybrid Monte Carlo
quantum dynamics

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10.1103/PhysRevApplied.22.L031004Licence: CC BY 4.0

Ostmeyer-etal-PRA-2024-First-principle-quantum-Monte-Carlo-study-of-charge-carrier-mobilityFinal published version, 1.27 MBLicence: CC BY 4.0

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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.",

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AB - 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.

KW - organic molecular semiconductors

KW - Hybrid Monte Carlo

KW - quantum dynamics

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

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