期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 12, 期 5, 页码 1490-1500出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.0c03314
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类别
资金
- EPSRC [EP/P012167/1]
- European Union [812872, 732013]
- EPSRC [EP/P012167/1] Funding Source: UKRI
The molecular photophysics and TADF mechanism in Spiro compounds are unique due to the rigid orthogonal C-C bridging bond between donor and acceptor. The photophysics process is highly complex, with unprecedented multiple anti-Kasha emissions from different singlet states, while the TADF mechanism is critically controlled by local acceptor n pi* states.
The molecular photophysics and thermally activated delayed fluorescence (TADF) in Spiro compounds are distinct because of the rigid orthogonal C-C bridging bond between donor and acceptor. The photophysics is found to be highly complex, with unprecedented multiple anti-Kasha emissions from three different singlet states, two of which are one-photon forbidden. The TADF mechanism is critically controlled by local acceptor n pi* states; the singlet n pi* state undergoes rapid intersystem crossing populating an energetically close acceptor pi pi* triplet state. The acceptor triplet n pi* state couples nonadiabatically to a CT triplet state mediating reverse intersystem crossing. When the n pi* and CT states are energetically close, TADF is greatly enhanced with rISC rate reaching 10(7) s(-1). We observe neither DF from the singlet n pi* state nor electron transfer (ET) to form the (CT)-C-1 because there is no ET driving force; however, ET from the higher-energy donor singlet pi pi* state readily occurs along with donor emission.
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