4.6 Review

Molecular Design Strategy for High-Yield and Long-Lived Individual Doubled Triplet Excitons through Intramolecular Singlet Fission

Journal

ACS ENERGY LETTERS
Volume 7, Issue 1, Pages 390-400

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.1c02300

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Funding

  1. JSPS KAKENHI [JP20H05832, JP21H05403, JP19H00888, JP20K21174, JP18H01957, JP18K19063, JP20H05234, JP20KK0120, JP21H01908, JP21K19011, JP20J13133]

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This review discusses the molecular design strategy for achieving high-yield and long-lived individual triplet exciton generation through intramolecular singlet fission, using a series of acene derivatives. It clarifies the structural and vibronic characters required for high-yield individual triplet exciton generation, and presents specific examples of photoenergy conversion far exceeding 100% quantum yields.
Multi-exciton generation of organic chromophores, i.e., singlet fission (SF), is highly promising for photoenergy conversion such as photocatalysis and photovoltaics. Among the reported high-yield SF systems, many systems possess only short-lived triplet excited states derived from correlated triplet pair intermediates, but not individual doubled triplet excitons. However, high-yield and long-lived individual triplet exciton generation is favorable for achieving efficient photoenergy conversion. In this Focus Review, we discuss the molecular design strategy for high-yield and long-lived individual triplet exciton generation through intramolecular SF utilizing a series of acene derivatives such as hexacene, pentacene, and tetracene. In addition to clarifying the structural and vibronic characters required for high-yield individual triplet exciton generation, specific examples of the photoenergy conversion far exceeding 100% quantum yields of subsequent electron-transfer products and singlet oxygen generation are presented.

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