Theoretical study on charge transfer properties of triphenylamino-ethynyl Polycyclic Aromatic Hydrocarbon derivatives

Fuente: arXiv
Salvato in:
Dettagli Bibliografici
Autori principali: Tong, Zhipeng, Sun, Xiaoqi, Qin, Guiya, Bai, Jinpu, Zhao, Qi, Ren, Aimin, Guo, Jingfu
Natura: Preprint
Pubblicazione: 2025
Soggetti:
Accesso online:
Tags: Aggiungi Tag
Nessun Tag, puoi essere il primo ad aggiungerne!!
_version_ 1866910969624526848
author Tong, Zhipeng
Sun, Xiaoqi
Qin, Guiya
Bai, Jinpu
Zhao, Qi
Ren, Aimin
Guo, Jingfu
author_facet Tong, Zhipeng
Sun, Xiaoqi
Qin, Guiya
Bai, Jinpu
Zhao, Qi
Ren, Aimin
Guo, Jingfu
contents This study systematically investigates the regulation mechanisms of backbone topology (tri-/tetracyclic arenes), substitution positions, and functional groups on charge transport properties through molecular design of triphenylamine-ethynylene fused acene derivatives. By integrating Marcus charge transfer theory with kinetic Monte Carlo simulations, we demonstrate that sulfur-doped tricyclic arene backbones (benzodithiophene and anthracene) effectively suppress high-frequency vibrational modes reducing reorganization energy to 146.1 meV. Concurrent optimization of intermolecular $π$-$π$ slippage enhances 2D hole mobility. Notably, asymmetric charge transport pathways in 2,7-disubstituted pyrene(27DTEP) decrease transfer integrals by 34%, while 1,6-substitution (16DTEP)reconstructs HOMO orbital distribution and induces rotational stacking, boosting transfer integrals by 28% and improving mobility isotropy. We further propose a "backbone-functional group synergy" strategy, revealing that concentrated orbital localization on the backbone amplifies transfer integral gains, outweighing the 38% increase in reorganization energy and significantly enhancing mobility. These findings establish a theoretical framework and quantitative model for the rational design of high-mobility organic ultraviolet photodetectors.
format Preprint
id arxiv_https___arxiv_org_abs_2505_20371
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Theoretical study on charge transfer properties of triphenylamino-ethynyl Polycyclic Aromatic Hydrocarbon derivatives
Tong, Zhipeng
Sun, Xiaoqi
Qin, Guiya
Bai, Jinpu
Zhao, Qi
Ren, Aimin
Guo, Jingfu
Chemical Physics
Computational Physics
This study systematically investigates the regulation mechanisms of backbone topology (tri-/tetracyclic arenes), substitution positions, and functional groups on charge transport properties through molecular design of triphenylamine-ethynylene fused acene derivatives. By integrating Marcus charge transfer theory with kinetic Monte Carlo simulations, we demonstrate that sulfur-doped tricyclic arene backbones (benzodithiophene and anthracene) effectively suppress high-frequency vibrational modes reducing reorganization energy to 146.1 meV. Concurrent optimization of intermolecular $π$-$π$ slippage enhances 2D hole mobility. Notably, asymmetric charge transport pathways in 2,7-disubstituted pyrene(27DTEP) decrease transfer integrals by 34%, while 1,6-substitution (16DTEP)reconstructs HOMO orbital distribution and induces rotational stacking, boosting transfer integrals by 28% and improving mobility isotropy. We further propose a "backbone-functional group synergy" strategy, revealing that concentrated orbital localization on the backbone amplifies transfer integral gains, outweighing the 38% increase in reorganization energy and significantly enhancing mobility. These findings establish a theoretical framework and quantitative model for the rational design of high-mobility organic ultraviolet photodetectors.
title Theoretical study on charge transfer properties of triphenylamino-ethynyl Polycyclic Aromatic Hydrocarbon derivatives
topic Chemical Physics
Computational Physics
url https://arxiv.org/abs/2505.20371