All-Atom Reactive Monte Carlo Molecular Dynamics for Molecular Doping in Organic Semiconductors.

IF 5.5 1区 化学 Q2 CHEMISTRY, PHYSICAL
Vishnu Raghuraman, Archana Verma, Nicholas E Jackson
{"title":"All-Atom Reactive Monte Carlo Molecular Dynamics for Molecular Doping in Organic Semiconductors.","authors":"Vishnu Raghuraman, Archana Verma, Nicholas E Jackson","doi":"10.1021/acs.jctc.5c01206","DOIUrl":null,"url":null,"abstract":"<p><p>The computational study of molecular doping in organic semiconductors (OSCs) is challenged by multiple competing length and time scales. We present an all-atom Reactive Monte Carlo Molecular Dynamics (RMCMD) method for quantitatively determining molecular doping efficiency in OSCs. A Metropolis criterion is employed for the doping reaction, which is parametrized from density functional theory (DFT) calculations of energetics and atomic partial charges of the doped and neutral molecular species. Polaronic effects are included in the RMCMD method to enable geometric reorganization upon doping, including the flattening of the inter-ring dihedrals. Extensions to partial charge transfer states are also developed to allow for the inclusion of charge transfer complexes. To demonstrate the validity of the approach, the doping efficiency and radial distribution function of a poly(3-hexylthiophene) system doped with 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane are calculated in an amorphous morphology. The method is implemented as a fix in LAMMPS, with the code made publicly available on GitHub.</p>","PeriodicalId":45,"journal":{"name":"Journal of Chemical Theory and Computation","volume":" ","pages":""},"PeriodicalIF":5.5000,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Chemical Theory and Computation","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.jctc.5c01206","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

Abstract

The computational study of molecular doping in organic semiconductors (OSCs) is challenged by multiple competing length and time scales. We present an all-atom Reactive Monte Carlo Molecular Dynamics (RMCMD) method for quantitatively determining molecular doping efficiency in OSCs. A Metropolis criterion is employed for the doping reaction, which is parametrized from density functional theory (DFT) calculations of energetics and atomic partial charges of the doped and neutral molecular species. Polaronic effects are included in the RMCMD method to enable geometric reorganization upon doping, including the flattening of the inter-ring dihedrals. Extensions to partial charge transfer states are also developed to allow for the inclusion of charge transfer complexes. To demonstrate the validity of the approach, the doping efficiency and radial distribution function of a poly(3-hexylthiophene) system doped with 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane are calculated in an amorphous morphology. The method is implemented as a fix in LAMMPS, with the code made publicly available on GitHub.

Abstract Image

有机半导体中分子掺杂的全原子反应蒙特卡罗分子动力学。
有机半导体(OSCs)中分子掺杂的计算研究受到多个竞争长度和时间尺度的挑战。我们提出了一种全原子反应性蒙特卡罗分子动力学(RMCMD)方法来定量测定osc中的分子掺杂效率。利用密度泛函理论(DFT)计算掺杂和中性分子的能量学和原子部分电荷,采用Metropolis准则对掺杂反应进行参数化。极化效应包括在RMCMD方法中,以实现掺杂后的几何重组,包括环间二面体的平坦化。扩展到部分电荷转移状态也被开发,以允许包含电荷转移配合物。为了证明该方法的有效性,在非晶形态下计算了掺杂2,3,5,6-四氟-7,7,8,8-四氰喹诺二甲烷的聚(3-己基噻吩)体系的掺杂效率和径向分布函数。该方法在LAMMPS中作为修复实现,其代码在GitHub上公开提供。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 求助全文
来源期刊
Journal of Chemical Theory and Computation
Journal of Chemical Theory and Computation 化学-物理:原子、分子和化学物理
CiteScore
9.90
自引率
16.40%
发文量
568
审稿时长
1 months
期刊介绍: The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信