期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 28, 页码 11591-11599出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202003560
关键词
charge transfer; electron spin control; intersystem crossing; time-resolved EPR; triplet state
资金
- NSFC [21673031, 21761142005, 21911530095, 21421005]
- State Key Laboratory of Fine Chemicals [ZYTS201901]
- Fundamental Research Funds for the Central Universities [DUT19TD28]
- SIBW/DFG
We prepared conceptually novel, fully rigid, spiro compact electron donor (Rhodamine B, lactam form, RB)/acceptor (naphthalimide; NI) orthogonal dyad to attain the long-lived triplet charge-transfer ((CT)-C-3) state, based on the electron spin control using spin-orbit charge transfer intersystem crossing (SOCT-ISC). Transient absorption (TA) spectra indicate the first charge separation (CS) takes place within 2.5 ps, subsequent SOCT-ISC takes 8 ns to produce the (NI)-N-3* state. Then the slow secondary CS (125 ns) gives the long-lived (CT)-C-3 state (0.94 mu s in deaerated n-hexane) with high energy level (ca. 2.12 eV). The cascade photophysical processes of the dyad upon photoexcitation are summarized as (NI)-N-1*->(CT)-C-1 ->(NI)-N-3*->(CT)-C-3. With time-resolved electron paramagnetic resonance (TREPR) spectra, an EEEAAA electron-spin polarization pattern was observed for the naphthalimide-localized triplet state. Our spiro compact dyad structure and the electron spin-control approach is different to previous methods for which invoking transition-metal coordination or chromophores with intrinsic ISC ability is mandatory.
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