Investigations reveal wavelength-dependent intramolecular singlet fission in contorted naphthalenediimide dimers, suggesting implications for photovoltaic efficiency.
Key Points
This research aims to explore the mechanistic details of singlet fission in rigid dimers and identify intermediates involved in this process.
Used polarization-controlled white-light two-dimensional spectroscopy and pump-probe spectroscopies
Investigated contorted naphthalenediimide dimers with favorable singlet fission pathways
Identified Davydov components and intermediate states through 2D cross-peaks and maps
Excitation of different Davydov components leads to the formation of a relaxed TT1 state
Intermediate formation is vibronically coherent with observable quantum beats in the TT1 photoproduct
Minimal electronic reorientation occurs during TT1 formation, maintaining significant mixing of singlet-triplet character