Citation: Qingxuan Fan, Wenjun Ni, Lingcheng Chen, Gagik G. Gurzadyan, Yi Xiao. Singlet relaxation dynamics and long triplet lifetimes of thiophene-coupled perylene diimides dyads: New insights for high efficiency organic solar cells[J]. Chinese Chemical Letters, ;2020, 31(11): 2965-2969. doi: 10.1016/j.cclet.2020.06.018 shu

Singlet relaxation dynamics and long triplet lifetimes of thiophene-coupled perylene diimides dyads: New insights for high efficiency organic solar cells

Qingxuan Fan ^{a, 1} ,
Wenjun Ni ^{b, 1} ,
Lingcheng Chen ^{a, *,} ,
Gagik G. Gurzadyan ^{b, *,} ,
Yi Xiao ^{a, *,}

a.
State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian 116024, China
b.
State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, Dalian University of Technology, Dalian 116024, China

lcchen@dlut.edu.cn

gurzadyan@dlut.edu.cn

xiaoyi@dlut.edu.cn

Received Date: 10 April 2020
Revised Date: 9 June 2020
Accepted Date: 10 June 2020
Available Online: 13 June 2020

Figures(5)

In the active layer of organic solar cells (OSCs), the lifetime of triplet excitons is one of the decisive factors in the diffusion length and therefore has important impact on the power conversion efficiency of the devices. Herein, we have investigated singlet excited state relaxation dynamics and their triplet exciton lifetimes of two thiophene-coupled perylene diimides (PDI) dyads (2PDI-Th and fused-2PDI-Th), in order to provide a unique explanation in depth on their different performances in OSC devices. From the transient absorption (TA) spectra, the singlet excitons of 2PDI-Th form excimers in the time scale of 1.5 ps. Then the excimers go into the triplet state via intersystem crossing (ISC). In fused-2PDI-Th, triplet excitons are generated directly from the singlet excited excitons via the efficient ISC. Density functional theory (DFT) calculations further support the formation of excimers. DFT results indicate that 2PDI-Th exhibits an H-typed molecular configuration which is beneficial to form the excimers, while fused-2PDI-Th gives a twisted X-shaped configuration in the optimized ground and excited state. In steady-state emission spectra, 2PDI-Th shows abroad and featureless spectral characteristics of the excimers with a decay time of 840 ps, which is much shorter than those of PDI (5.5 ns) and fused-2PDI-Th (3.3 ns). The triplet lifetime (67 μs) of fused-2PDI-Th is factor of 3 longer than that of 2PDI-Th (22 μs). These results demonstrate that ring-fused structure is an efficient strategy to eliminate excimer formation and prolong the lifetime of triplet excitons, which provides a new insight for design of optoelectronic molecules for high efficiency organic solar cells.
- Ultrafast relaxation dynamics,
- Triplet excited state,
- Exciton lifetime,
- Photophysical process,
- Organic solar cell
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