期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 2, 页码 2887-2898出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c15893
关键词
quinoid-aromatic conjugated polymers; closed-shell quinoidal and open-shell diradical structures; charge transport; OFET; spin characteristics
资金
- Samsung Research Funding & Incubation Center of Samsung Electronics [SRFC-MA1802-03]
- National Research Foundation of Korea (NRF) - Korea Government [NRF-2018R1A2A1A05078791]
This work successfully demonstrated how the control of the closed/open-shell character of quinoidal building blocks changes charge transport and spin properties of quinoidal conjugated polymers via quinoid-aromatic interconversion.
While quinoidal moieties are considered as emerging platforms showing efficient charge transport and interesting open-shell diradical characteristics, whether these properties could be changed by extension to the conjugated polymer structure remains as a fundamental question. Here, we developed and characterized two conjugated polymers incorporating quinoids with different lengths, which have a stable close- and open-shell diradical character, respectively, namely, poly(quinoidal thiophene-thienylene vinylene) (PQuT-TV) and poly(quinoidal bithiophene-thienylene vinylene) (PQuBT-TV). A longer length of a quinoidal core led to enhanced diradical characteristics. Therefore, the longer core length of QuBT was favorable for the formation of an open-shell diradical structure in its monomer and in the quinoidal polymer. PQuBT-TV exhibited high spin characteristics observed by the strong ESR signal, a low band gap, and improved electrochemical stability. On the other hand, as QuT maintained a closed-shell quinoid structure, PQuT-TV exhibited high backbone coplanarity and strong intermolecular interaction, which was beneficial for charge transport and led to high hole mobility (up to 2.40 cm(2) V-1 s(-1)) in organic field-effect transistors. This work successfully demonstrated how the control of the closed/open-shell character of quinoidal building blocks changes charge transport and spin properties of quinoidal conjugated polymers via quinoid-aromatic interconversion.
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