Unraveling the Impact of Non-Covalent Interactions and Different Donor Moieties on Charge Transport in DPPT-Based Polymers
Year: 2025
Author: Jinyang Luo, Jiawei Dong, Guo Wang, Linjun Wang, Hua Geng
Communications in Computational Chemistry, Vol. 7 (2025), Iss. 2 : pp. 111–119
Abstract
The integration of both rigid and flexible components holds great potential to significantly enhance the overall performance of organic electronic devices. Non-covalent interactions are frequently harnessed to augment the planar conjugation of polymers, consequently elevating the rigidity of these polymers. However, the influence of the dihedral angle distortion between donor and acceptor units, which is induced by the flexibility inherent in donor-acceptor copolymers, on charge transport remains poorly understood. In this study, we systematically investigate intra-chain charge transport parameters and charge mobility for the 3,6-bis(thiophen-2-yl) diketopyrrolopyrrole (DPPT) conjugated with various donor moieties. Combining with density functional theory (DFT) and the Su-Schrieffer-Heeger (SSH) model, we find that when the non-covalent interactions between the donor and acceptor units are enhanced (as exemplified by DPPT-FT and DPPT-BO), the coupling between electrons and low-frequency vibrations is significantly suppressed. Simultaneously, the intra-chain electronic coupling increases owing to substantial orbital overlap. Surface hopping simulations are utilized to study the charge transport properties. For DPPT-T, DPPT-FT, and DPPT-BT, weaker molecular rigidity and disordered chain packing lead to thermally activated hopping transport (low electronic coupling and high reorganization energy). In contrast, the enhanced structural rigidity of DPPT-BO facilitates charge delocalization, leading to an initial improvement in carrier mobility under low-temperature conditions, and thermal fluctuation effects induce a band-like behavior at high temperature.
Journal Article Details
Publisher Name: Global Science Press
Language: English
DOI: https://doi.org/10.4208/cicc.2025.80.01
Communications in Computational Chemistry, Vol. 7 (2025), Iss. 2 : pp. 111–119
Published online: 2025-01
AMS Subject Headings: Global Science Press
Copyright: COPYRIGHT: © Global Science Press
Pages: 9
Keywords: charge transport Diketopyrrolopyrrole copolymers torsional stiffness non-covalent interactions Su-Schrieffer-Heeger model.