Singlet Fission Dynamics of Colloidal Nanoparticles of a Perylenediimide Derivative in Solutions.

Singlet fission (SF) is an intriguing process in which a singlet exciton produces two triplet excitons in molecular aggregates. Perylenediimide (PDI) derivatives are promising materials for SF-based photovoltaics, and the SF process in PDI aggregates is important to investigate for their applications. In this work, we studied the entire SF process occurring in the colloidal nanoparticles of a PDI derivative in solutions by using time-resolved fluorescence and transient absorption (TA) experiments. PE-PDI was found to form the colloidal nanoparticles of H- and J-aggregates in polar solvents. The TA signals of PE-PDI aggregates in solutions were selectively measured by wavelength-dependent excitation. The TA signals were analyzed by using a global fitting analysis, and all kinetic parameters involved in the entire SF process were determined. Our current investigation has confirmed that fast SF occurs on the surface of the colloidal nanoparticles of PDI aggregates via the charge transfer mediated mechanism, giving a high quantum yield of triplet excitons.