Dynamical aspects of excitonic Floquet states generated by a phase-locked mid-infrared pulse in a one-dimensional Mott insulator

Abstract

A periodic electric field of light applied on a solid is predicted to generate coupled states of the light electric fields and electronic system called photon-dressed Floquet states. Previous studies of those Floquet states have focused on time-averaged energy-level structures. Here, we report time-dependent responses of Floquet states of excitons generated by a mid-infrared (MIR) pulse excitation in a prototypical one-dimensional (1D) Mott insulator, a chlorine-bridged nickel-chain compound, [Ni(chxn)2Cl](NO3)2 (chxn = cyclohexanediamine). Sub-cycle reflection spectroscopy on this compound using a phase-locked MIR pump pulse and an ultrashort visible probe pulse with the temporal width of ∼7 fs revealed that large and ultrafast reflectivity changes occur along the electric field of the MIR pulse; the reflectivity change reached approximately 50% of the original value around the exciton absorption peak. It comprised a high-frequency oscillation at twice the frequency of the MIR pulse and a low-frequency component following the intensity envelope of the MIR pulse, which showed different probe-energy dependences. Simulations considering one-photon-allowed and one-photon-forbidden excitons reproduced the temporal and spectral characteristics of both the high-frequency oscillation and low-frequency component. These simulations demonstrated that all responses originated from the quantum interferences of the linear reflection process and nonlinear light-scattering processes owing to the excitonic Floquet states characteristic of 1D Mott insulators. The present results lead to the developments of Floquet engineering, and demonstrate the possibility of rapidly controlling the intensity of visible or near-IR pulse by varying the phase of MIR electric fields, which will be utilized for ultrafast optical switching devices.