有机分子半导体中电荷载流子迁移率的第一原理量子蒙特卡洛研究

IF 3.8 2区物理与天体物理 Q2 PHYSICS, APPLIED

Physical Review Applied Pub Date : 2024-09-10 DOI:10.1103/physrevapplied.22.l031004

Johann Ostmeyer, Tahereh Nematiaram, Alessandro Troisi, Pavel Buividovich

{"title":"有机分子半导体中电荷载流子迁移率的第一原理量子蒙特卡洛研究","authors":"Johann Ostmeyer, Tahereh Nematiaram, Alessandro Troisi, Pavel Buividovich","doi":"10.1103/physrevapplied.22.l031004","DOIUrl":null,"url":null,"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 <math display=\"inline\" overflow=\"scroll\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mrow><mrow><mi mathvariant=\"script\">O</mi></mrow></mrow><mo></mo><mrow><mo>(</mo><mn>1</mn><mo>)</mo></mrow></mrow></math> CPU hours. Our simulations produce charge-mobility estimates that are in good agreement with experiments and that also justify the phenomenological transient localization approach.","PeriodicalId":20109,"journal":{"name":"Physical Review Applied","volume":"59 1","pages":""},"PeriodicalIF":3.8000,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"First-principles quantum Monte Carlo study of charge-carrier mobility in organic molecular semiconductors\",\"authors\":\"Johann Ostmeyer, Tahereh Nematiaram, Alessandro Troisi, Pavel Buividovich\",\"doi\":\"10.1103/physrevapplied.22.l031004\",\"DOIUrl\":null,\"url\":null,\"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 <math display=\\\"inline\\\" overflow=\\\"scroll\\\" xmlns=\\\"http://www.w3.org/1998/Math/MathML\\\"><mrow><mrow><mrow><mi mathvariant=\\\"script\\\">O</mi></mrow></mrow><mo></mo><mrow><mo>(</mo><mn>1</mn><mo>)</mo></mrow></mrow></math> CPU hours. Our simulations produce charge-mobility estimates that are in good agreement with experiments and that also justify the phenomenological transient localization approach.\",\"PeriodicalId\":20109,\"journal\":{\"name\":\"Physical Review Applied\",\"volume\":\"59 1\",\"pages\":\"\"},\"PeriodicalIF\":3.8000,\"publicationDate\":\"2024-09-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Physical Review Applied\",\"FirstCategoryId\":\"101\",\"ListUrlMain\":\"https://doi.org/10.1103/physrevapplied.22.l031004\",\"RegionNum\":2,\"RegionCategory\":\"物理与天体物理\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"PHYSICS, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Physical Review Applied","FirstCategoryId":"101","ListUrlMain":"https://doi.org/10.1103/physrevapplied.22.l031004","RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"PHYSICS, APPLIED","Score":null,"Total":0}

引用次数: 0

摘要

我们介绍了对有机分子半导体二维紧密结合模型中电荷传输的第一原理数值研究。我们使用混合蒙特卡洛（HMC）算法模拟声子和单个或多个电荷载流子的全部量子动力学，而无需任何可调参数。我们引入了一系列算法改进，包括基于分析见解的声子场高效 Metropolis 更新，这使得自相关时间可以忽略不计，并能以 O(1) 个 CPU 小时的低计算成本达到亚微米精度。我们的模拟得出的电荷流动性估计值与实验结果非常吻合，也证明了现象学瞬态定位方法的正确性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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

查看原文本刊更多论文

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

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.

求助全文

通过发布文献求助，成功后即可免费获取论文全文。去求助

来源期刊

Physical Review Applied PHYSICS, APPLIED-

CiteScore

7.80

自引率

8.70%

发文量

760

审稿时长

2.5 months

期刊介绍： Physical Review Applied (PRApplied) publishes high-quality papers that bridge the gap between engineering and physics, and between current and future technologies. PRApplied welcomes papers from both the engineering and physics communities, in academia and industry. PRApplied focuses on topics including: Biophysics, bioelectronics, and biomedical engineering, Device physics, Electronics, Technology to harvest, store, and transmit energy, focusing on renewable energy technologies, Geophysics and space science, Industrial physics, Magnetism and spintronics, Metamaterials, Microfluidics, Nonlinear dynamics and pattern formation in natural or manufactured systems, Nanoscience and nanotechnology, Optics, optoelectronics, photonics, and photonic devices, Quantum information processing, both algorithms and hardware, Soft matter physics, including granular and complex fluids and active matter.