Abstract

Mott insulators sometimes show dramatic changes in their electronic states after photoirradiation, as indicated by photoinduced Mott-insulator-to-metal transition. In the photoexcited states of Mott insulators, electron wave functions are more delocalized than in the ground state, and long-range Coulomb interactions play important roles in charge dynamics. However, their effects are difficult to discriminate experimentally. Here, we show that in a one-dimensional Mott insulator, bis(ethylenedithio)tetrathiafulvalene-difluorotetracyanoquinodimethane (ET-F₂TCNQ), long-range Coulomb interactions stabilize not only excitons, doublon-holon bound states, but also biexcitons. By measuring terahertz-electric-field-induced reflectivity changes, we demonstrate that odd- and even-parity excitons are split off from a doublon-holon continuum. Further, spectral changes of reflectivity induced by a resonant excitation of the odd-parity exciton reveals that an exciton-biexciton transition appears just below the exciton-transition peak. Theoretical simulations show that long-range Coulomb interactions over four sites are necessary to stabilize the biexciton. Such information is indispensable for understanding the non-equilibrium dynamics of photoexcited Mott insulators.

Papers

T. Miyamoto, T. Kakizaki, T. Terashige, D. Hata, H. Yamakawa, T. Morimoto, N. Takamura, H. Yada, Y. Takahashi, T. Hasegawa, H. Matsuzaki, T. Tohyama, and H. Okamoto,"Biexciton in one-dimensional Mott insulators",Communications Physics,10.1038/s42005-019-0223-8