Competing Trion and Exciton Dynamics in a Quasi-One-Dimensional Correlated Semiconductor

Abstract: Strong Coulomb interactions in low-dimensional quantum materials give rise to emergent bound states such as excitons and trions, which play a central role in correlated electronic phases. In quasi-one-dimensional systems, equilibrium photoemission studies have reported signatures of trions, suggesting an unusually robust state, as opposed to conventional semiconductors where trions typically appear only as excited states stabilized by carrier doping. Here, we show that optical excitation of undoped Ta2NiS5 - a correlated quasi-one-dimensional semiconductor - generates a pronounced and long-lived trion population, demonstrating that such states can be dynamically induced even in the absence of doping. Using time- and angle-resolved photoemission spectroscopy we track the dynamics of a bright, localized in-gap state that emerges following photoexcitation and identify it as a transient trion population. We uncover an unconventional trion formation pathway and a fluence-dependent competition between trions and excitons. These findings extend ultrafast quasiparticle photoemission spectroscopy to complex bound states in bulk quantum materials, enabling the dynamical control of charged and neutral excitations.