Towards multistate multimode landscapes in singlet fission of pentacene: the dual role of charge-transfer states.

ABSTRACT: Singlet fission duplicates triplet excitons for improving light harvesting efficiency. The presence of the interaction between electronic and nuclear degrees of freedom complicates the interpretation of correlated triplet pairs. We report a quantum chemistry study on the significance and subtleties of multistate and multimode pathways in forming triplet pair states of the pentacene dimer through a six-state vibronic-coupling Hamiltonian derived from many-electron adiabatic wavefunctions of an ab initio density matrix renormalization group. The resulting spin values of the singlet manifolds on each pentacene center are computed, and the varying spin nature can be distinguished clearly with respect to dimer stacking and vibronic progression. Our monomer spin assignments reveal the coe

SUBMITTER: Walia R 

PROVIDER: S-EPMC8514007 | biostudies-literature | 2021 Oct

REPOSITORIES: biostudies-literature