TY - JOUR
T1 - Controlled Orientations of Neighboring Tetracene Units by Mixed Self-Assembled Monolayers on Gold Nanoclusters for High-Yield and Long-Lived Triplet Excited States through Singlet Fission
AU - Saegusa, Toshiyuki
AU - Sakai, Hayato
AU - Nagashima, Hiroki
AU - Kobori, Yasuhiro
AU - Tkachenko, Nikolai V.
AU - Hasobe, Taku
N1 - Funding Information:
This work was partially supported by JSPS KAKENHI Grant Numbers JP18H01957, 18K19063, 17H05270, and 17H05162 to T.H., 19H00888, 17K19105, and 16H04097 to Y.K., 17J01125 to H.N., and 17K14476 to H.S. This work was carried out by the joint research program of Molecular Photoscience Research Center, Kobe University. We also thank Prof. H. Tsunoyama (Keio Univ.) for useful suggestions and discussion regarding XRD measurements.
Funding Information:
This work was partially supported by JSPS KAKENHI Grant Numbers JP18H01957, 18K19063, 17H05270, and 17H05162 to T.H. 19H00888, 17K19105, and 16H04097 to Y.K., 17J01125 to H.N., and 17K14476 to H.S. This work was carried out by the joint research program of Molecular Photoscience Research Center, Kobe University. We also thank Prof. H. Tsunoyama (Keio Univ.) for useful suggestions and discussion regarding XRD measurements.
Publisher Copyright:
Copyright © 2019 American Chemical Society.
PY - 2019/9/18
Y1 - 2019/9/18
N2 - Although tetracene (Tc) is well-known as a good candidate for singlet fission (SF), the number of high-yield and long-lived triplet excited states through SF is extremely limited because of the relative acceleration of the reverse triplet-triplet annihilation (TTA) considering the energy matching between a singlet and two triplet states. Systematic control of electronic interactions between two neighboring units using conventional covalent linkages and molecular assembly methods to optimize these kinetic processes is quite difficult because of the complicated synthesis and random orientations. In this study, we propose a novel supramolecular strategy utilizing mixed self-assembled monolayers (SAMs) with two different chain lengths. Specifically, mixed Tc-SAMs on gold nanoclusters, which are prepared using Tc-modified heterodisulfides with two different chain lengths, attain high-yield SF (φSF ≈ 90%) and individual triplet yields (φ? ≈ 160%). The obtained φSF is the highest value among Tc derivatives in homogeneous solution to the best of our knowledge.
AB - Although tetracene (Tc) is well-known as a good candidate for singlet fission (SF), the number of high-yield and long-lived triplet excited states through SF is extremely limited because of the relative acceleration of the reverse triplet-triplet annihilation (TTA) considering the energy matching between a singlet and two triplet states. Systematic control of electronic interactions between two neighboring units using conventional covalent linkages and molecular assembly methods to optimize these kinetic processes is quite difficult because of the complicated synthesis and random orientations. In this study, we propose a novel supramolecular strategy utilizing mixed self-assembled monolayers (SAMs) with two different chain lengths. Specifically, mixed Tc-SAMs on gold nanoclusters, which are prepared using Tc-modified heterodisulfides with two different chain lengths, attain high-yield SF (φSF ≈ 90%) and individual triplet yields (φ? ≈ 160%). The obtained φSF is the highest value among Tc derivatives in homogeneous solution to the best of our knowledge.
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U2 - 10.1021/jacs.9b06567
DO - 10.1021/jacs.9b06567
M3 - Article
C2 - 31529955
AN - SCOPUS:85072270985
SN - 0002-7863
VL - 141
SP - 14720
EP - 14727
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 37
ER -