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Singlet fission of hot excitons in ?-conjugated polymers #MMPMID25987576
Zhai Y; Sheng C; Vardeny ZV
Philos Trans A Math Phys Eng Sci 2015[Jun]; 373 (2044): ä PMID25987576show ga
We used steady-state photoinduced absorption (PA), excitation dependence (EXPA(?)) spectrum of the triplet exciton PA band, and its magneto-PA (MPA(B)) response to investigate singlet fission (SF) of hot excitons into two separated triplet excitons, in two luminescent and non-luminescent ?-conjugated polymers. From the high energy step in the triplet EXPA(?) spectrum of the luminescent polymer poly(dioctyloxy)phenylenevinylene (DOO-PPV) films, we identified a hot-exciton SF (HE-SF) process having threshold energy at E?2ET (=2.8?eV, where ET is the energy of the lowest lying triplet exciton), which is about 0.8?eV above the lowest singlet exciton energy. The HE-SF process was confirmed by the triplet MPA(B) response for excitation at E>2ET, which shows typical SF response. This process is missing in DOO-PPV solution, showing that it is predominantly interchain in nature. By contrast, the triplet EXPA(?) spectrum in the non-luminescent polymer polydiacetylene (PDA) is flat with an onset at E=Eg (?2.25?eV). From this, we infer that intrachain SF that involves a triplet?triplet pair state, also known as the ?dark? 2Ag exciton, dominates the triplet photogeneration in PDA polymer as Eg>2ET. The intrachain SF process was also identified from the MPA(B) response of the triplet PA band in PDA. Our work shows that the SF process in ?-conjugated polymers is a much more general process than thought previously.