Singlet Fission in a para-Azaquinodimethane-Based Quinoidal Conjugated Polymer

Wang, Long; Liu, Xuncheng; Shi, Xiaomei; Anderson, Christopher L.; Klivansky, Liana M.; Liu, Yi; Wu, Yishi; Chen, Junwu; Yao, Jiannian; Fu, Hongbing

doi:10.1021/jacs.0c06604

Singlet Fission in a para-Azaquinodimethane-Based Quinoidal Conjugated Polymer

Journal Article · Mon Oct 12 00:00:00 EDT 2020 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.0c06604· OSTI ID:1834565

^[1]; ^[2]; Shi, Xiaomei ^[3]; Anderson, Christopher L. ^[4]; Klivansky, Liana M. ^[5]; ^[5]; Wu, Yishi ^[6]; ^[7]; Yao, Jiannian ^[8]; ^[6]

Taiyuan Univ. of Technology (China)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); South China Univ. of Technology, Guangzhou (China); Guizhou Univ. (China)
Shanxi Medical Univ., Taiyuan (China)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Capital Normal Univ., Beijing (China)
South China Univ. of Technology, Guangzhou (China)
Chinese Academy of Sciences, Beijing (China)

The exploitation of singlet fission (SF) in photovoltaic devices is restricted by the limited number of SF materials available and the conflicting requirement of intermolecular interactions to satisfy both efficient SF and subsequent triplet extraction. Intramolecular SF (iSF) represents an emerging alternative and may prove simpler to implement in devices. Here, on account of the excellent chemical structure tunability and solution processability, conjugated polymers have emerged as promising candidates for iSF materials despite being largely underexplored. It remains a significant challenge to develop SF-capable conjugated polymers and achieve efficient dissociation of the formed triplet pairs simultaneously. In this contribution, we present a new iSF material in a para-azaquinodimethane-based quinoidal conjugated polymer. Using transient optical techniques, we show that an ultrafast iSF process dominates the deactivation of the excited state in such polymer, featuring ultrafast population (<1 ps) and stepwise dissociation of triplet pairs. Notably, these multiexciton states could further diffuse apart to produce long-lived free triplets (tens of μs) in strongly coupled aggregates in solid thin film. Such findings not only introduce a new iSF-active conjugated polymer to the rare SF material family but also shed unique insight into interchain interaction-promoted triplet pair dissociation in aggregates of conjugated polymers, thus openning new avenues for developing next-generation SF-based photovoltaic materials.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1834565

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 42 Vol. 142; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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