Biexciton in one-dimensional Mott insulators
arXiv:1907.13338 · doi:10.1038/s42005-019-0223-8
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 wavefunctions 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.
30 pages including 4 figures and 1 table (Supplementary Informations: 8 pages including 5 figures)
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