期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 49, 页码 22179-22184出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202009439
关键词
charge-transfer states; SOCT-ISC; spiro conjugation; triplet states; triplet quantum yields
资金
- National Nature Science Foundation of China [91850202, 21873030, 11674101, 21574039, 20822805]
- Shanghai Rising-Star Program [19QA1402800]
- Shanghai Municipal Science and Technology Commission [18DZ1112703]
- Spanish Government MINECO/FEDER [PID2019-109555GB-I00]
- Basque Government [PIBA19-0004]
- CONACYT-Mexico for a Ph.D. fellowship [591700]
Spiro conjugation has been proposed to dictate the efficiency of charge transfer, which could directly affect the spin-orbit charge transfer intersystem crossing (SOCT-ISC) process. However, this process has yet to be exemplified. Herein, we prepared three spirobis[anthracene]diones, in which two benzophenone moieties are locked in close proximity and differentially functionalized to fine-tune the charge transfer state. Its feasibility for SOCT-ISC was theoretically predicted, then experimentally evaluated. Through fine-tuning the spiro conjugation coupling and varying the solvent dielectric constants, ISC rate constants were engineered to vary in a dynamic range of three orders of magnitude, from 7.8x10(8) s(-1)to 1.0x10(11) s(-1), which is the highest ISC rate reported for SOCT-ISC system to our knowledge. Our findings substantiate the key factors for effective SOCT-ISC and offer a new avenue for the rational design of heavy atom free triplet sensitizers.
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