Biexciton in one-dimensional Mott insulators

TL;DR

This paper demonstrates that long-range Coulomb interactions in a one-dimensional Mott insulator stabilize biexcitons, with experimental and theoretical evidence showing their formation and spectral signatures, advancing understanding of photoexcited states.

Contribution

It reveals the role of long-range Coulomb interactions in stabilizing biexcitons in a 1D Mott insulator through combined experimental and theoretical analysis.

Findings

Long-range Coulomb interactions stabilize biexcitons.

Spectral evidence of exciton-biexciton transition.

Theoretical simulations confirm the necessity of four-site interactions.

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.