Coherent optical response driven by non-equilibrium electron–phonon dynamics in a layered transition-metal dichalcogenide

Abstract

Layered transition-metal dichalcogenides (TMDs) are model systems to explore ultrafast many-body interactions and various nonlinear optical phenomena. For the application of TMD-based optoelectronic devices capable of ultrafast response, it is essential to understand how characteristic electron–hole and electron–phonon couplings modify ultrafast electronic and optical properties under photoexcitation. Here, we investigate the sub-picosecond optical responses of layered semiconductor 2H–MoTe2 in the presence of an electron–hole (e–h) plasma and a long-lived coherent phonon. Transient reflectivity measurements depending on photon energy reveal that the optical response for short-time delays (< 1ps) was significantly modified by band-gap renormalization and state filling due to the presence of the e–h plasma. Furthermore, octave, sum, and difference phonon frequencies transiently appeared for the early time delays (< 2ps). The emergent multiple phonon frequencies can be described as higher-order optical modulations due to deformation-potential electron–phonon coupling under resonant photoexcitation conditions. This work provides comprehensive insights into fundamental physics and the application of non-equilibrium quasiparticle generations on TMDs under time-periodic phonon driving forces.