TY - JOUR
T1 - Near-Unity Singlet Fission on a Quantum Dot Initiated by Resonant Energy Transfer
AU - Zhang, Jie
AU - Sakai, Hayato
AU - Suzuki, Katsuaki
AU - Hasobe, Taku
AU - Tkachenko, Nikolai V.
AU - Chang, I. Ya
AU - Hyeon-Deuk, Kim
AU - Kaji, Hironori
AU - Teranishi, Toshiharu
AU - Sakamoto, Masanori
N1 - Funding Information:
We thank Unisoku Co. Ltd. and Tatsuo Nakagawa for their contribution to time-resolved fluorescence measurements. This study was supported by KAKENHI 18H01827 (Grant-in-Aid for Scientific Research (B)), 21H04638 (Grant-in-Aid for Scientific Research (A) (M.S.), 20K05652 (Grant-in-Aid for Scientific research (C)) (H.S.), 20KK0120 (Fostering Joint International Research (B)) (T.H.), JP16H06520 (Coordination Asymmetry) (H.S. and T.T.), JP17H05257 (Photosynergetics) (M.S. and T.H.), JST FOREST Program, JPMJFR201M (JST FOREST Program) (M.S.), and 19J14834 (JSPS Research Fellowship) (J.Z.).
Publisher Copyright:
© 2021 American Chemical Society.
PY - 2021/10/27
Y1 - 2021/10/27
N2 - The conversion of a high-energy photon into two excitons using singlet fission (SF) has stimulated a variety of studies in fields from fundamental physics to device applications. However, efficient SF has only been achieved in limited systems, such as solid crystals and covalent dimers. Here, we established a novel system by assembling 4-(6,13-bis(2-(triisopropylsilyl)ethynyl)pentacen-2-yl)benzoic acid (Pc) chromophores on nanosized CdTe quantum dots (QDs). A near-unity SF (198 ± 5.7%) initiated by interfacial resonant energy transfer from CdTe to surface Pc was obtained. The unique arrangement of Pc determined by the surface atomic configuration of QDs is the key factor realizing unity SF. The triplet-triplet annihilation was remarkably suppressed due to the rapid dissociation of triplet pairs, leading to long-lived free triplets. In addition, the low light-harvesting ability of Pc in the visible region was promoted by the efficient energy transfer (99 ± 5.8%) from the QDs to Pc. The synergistically enhanced light-harvesting ability, high triplet yield, and long-lived triplet lifetime of the SF system on nanointerfaces could pave the way for an unmatched advantage of SF.
AB - The conversion of a high-energy photon into two excitons using singlet fission (SF) has stimulated a variety of studies in fields from fundamental physics to device applications. However, efficient SF has only been achieved in limited systems, such as solid crystals and covalent dimers. Here, we established a novel system by assembling 4-(6,13-bis(2-(triisopropylsilyl)ethynyl)pentacen-2-yl)benzoic acid (Pc) chromophores on nanosized CdTe quantum dots (QDs). A near-unity SF (198 ± 5.7%) initiated by interfacial resonant energy transfer from CdTe to surface Pc was obtained. The unique arrangement of Pc determined by the surface atomic configuration of QDs is the key factor realizing unity SF. The triplet-triplet annihilation was remarkably suppressed due to the rapid dissociation of triplet pairs, leading to long-lived free triplets. In addition, the low light-harvesting ability of Pc in the visible region was promoted by the efficient energy transfer (99 ± 5.8%) from the QDs to Pc. The synergistically enhanced light-harvesting ability, high triplet yield, and long-lived triplet lifetime of the SF system on nanointerfaces could pave the way for an unmatched advantage of SF.
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U2 - 10.1021/jacs.1c04731
DO - 10.1021/jacs.1c04731
M3 - Article
C2 - 34647732
AN - SCOPUS:85118242750
SN - 0002-7863
VL - 143
SP - 17388
EP - 17394
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 42
ER -