No abstract

No abstract

In an electronic system of solids excited by a femtosecond laser pulse, new quantum states called photon-dressed states are created via the coupling of original electron wavefunctions and periodic electric fields of light. The study of photon-dressed states is a central issue in nonlinear optical science, as a coherent response associated with a photon-dressed state can cause ultrafast optical-switching phenomena. In general, however, phase-sensitive dynamics of photon-dressed states are difficult to observe due to their short lifetime. Here, we show that excitation of the organic Mott insulator potassium-tetracyanoquinodimethane with a strong mid-infrared pulse induces a couple of intramolecular vibrations, which add temporally periodic potentials to the electronic system, giving rise to phonon-dressed states in the picosecond time domain. Through sub-cycle spectroscopy using a phase-stable mid-infrared pulse as an excitation and an ultrashort visible pulse as a probe, we observe optical radiation consisting of four kinds of coherent oscillations with double, sum, and differential frequencies of two intramolecular vibrations. The probe-energy dependence of each oscillation can be well interpreted with phonon-dressed states in the framework of Floquet theory. These findings open a possibility for Floquet engineering in correlated electron materials with strong charge–phonon couplings.