Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 27, Issue 4, Pages 1337-1345Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.202002862
Keywords
charge transfer; density functional calculations; donor– acceptor systems; femtochemistry; luminescence
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Funding
- National Natural Science Foundation of China [21773151]
- STU Scientific Research Foundation for Talents [130-760189]
- Educational Commission of Guangdong Province of China [2019KCXTD007]
- Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme 2019 [GDUPS2019]
- Guangdong-Hong Kong-Macau Greater Bay Area Joint Breeding Laboratory [130/18219470]
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Two deep-blue luminescent materials were designed using the bipolarity of 1,2-diphenylphenanthroimidazole, with investigation of their excited-state evolution and interchromophoric interactions revealing factors such as electronic nature, structure, and solvent polarity influencing intramolecular charge transfer lifetime.
By utilizing the bipolarity of 1,2-diphenylphenanthroimidazole (PPI), two types of asymmetrical tripartite triads (PPI-TPA and PPI-PCz) were designed with triphenylamine (TPA) and 9-phenylcarbazole (PCz). These triads are deep-blue luminescent materials with a high fluorescence quantum yield of nearly 100 %. To trace the photophysical behaviors of these triads, their excited-state evolution channels and interchromophoric interactions were investigated by ultrafast time-resolved transient absorption and excited-state theoretical calculations. The results suggest that the electronic nature, asymmetrical tripartite structure, and electron-hole distance of these triads, as well as solvent polarity, determine the lifetime of intramolecular charge transfer (ICT). Interestingly, PPI-PCz triads show anti-Kasha ICT, and the charge-transfer direction among the triads is adjustable. For the PPI-TPA triad, the electron is transferred from TPA to PPI, whereas for the PPI-PCz triad the electron is pushed from PPI to PCz. Exploration of the excited-state ICT in these triads may pave the way to design better luminescent materials in the future.
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