Excitonic switching across a Z2 topological phase transition: From Mott-Wannier to Frenkel excitons in organic materials

Abstract

Controllable topological phase transitions are appealing as they allow for tunable single particle electronic properties. Here, by using state-of-the-art manybody perturbation theory techniques, we show that the topological $Z_2$ phase transition occurring in the single particle spectrum of the recently synthetized ethynylene bridged polyacene polymers is accompanied by a topological excitonic phase transition: the band inversion in the non-trivial phase yields real-space exciton wave functions in which electrons and holes exchange orbital characters with respect to the trivial phase. The topological excitonic phase transition results in a broad tunability of the singlet-triplet splittings, opening appealing perspectives for the occurrence of singlet fission. Finally, the flatness of the single-particle electronic structure in the topological non trivial phase leads to negatively dispersing triplet excitons in a large portion of the Brillouin zone, opening a route for spontaneously coherent energy transport at room temperature.