Exciton Diffusion in Highly-Ordered One Dimensional Conjugated Polymers: Effects of Back-Bone Torsion, Electronic Symmetry, Phonons and Annihilation

被引:13
作者
Pandya, Raj [1 ]
Alvertis, Antonios M. [1 ]
Gu, Qifei [1 ]
Sung, Jooyoung [1 ]
Legrand, Laurent [2 ]
Kreher, David [3 ]
Barisien, Thierry [2 ]
Chin, Alex W. [2 ]
Schnedermann, Christoph [1 ]
Rao, Akshay [1 ]
机构
[1] Univ Cambridge, Cavendish Lab, Cambridge CB3 0HE, England
[2] Sorbonne Univ, Inst NanoSci Paris, INSP, CNRS, F-75005 Paris, France
[3] Sorbonne Univ, Inst Parisien Chim Mol IPCM UMR 8232, Chim Polymeres, CNRS, F-75005 Paris, France
基金
英国工程与自然科学研究理事会;
关键词
ISOLATED POLYDIACETYLENE CHAINS; TEMPERATURE-DEPENDENCE; SINGLET FISSION; STATE; TRANSPORT;
D O I
10.1021/acs.jpclett.1c00193
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Many optoelectronic devices based on organic materials require rapid and long-range singlet exciton transport. Key factors controlling exciton transport include material structure, exciton-phonon coupling and electronic state symmetry. Here, we employ femtosecond transient absorption microscopy to study the influence of these parameters on exciton transport in one-dimensional conjugated polymers. We find that excitons with 2(1)A(g)(-) symmetry and a planar backbone exhibit a significantly higher diffusion coefficient (34 +/- 10 cm(2) s(-1)) compared to excitons with 1(1)B(u)(+) symmetry (7 +/- 6 cm(2) s(-1)) with a twisted backbone. We also find that exciton transport in the 2(1)Ag(-) state occurs without exciton-exciton annihilation. Both 2(1)A(g)(-) and 1(1)Bu(+) states are found to exhibit subdiffusive behavior. Ab initio GW-BSE calculations reveal that this is due to the comparable strengths of the exciton-phonon interaction and exciton coupling. Our results demonstrate the link between electronic state symmetry, backbone torsion and phonons in exciton transport in pi-conjugated polymers.
引用
收藏
页码:3669 / 3678
页数:10
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