Transient field-resolved reflectometry at 50-100 THz

TL;DR

This paper extends transient field-resolved spectroscopy to 50-100 THz, enabling ultrafast studies of materials with sub-cycle resolution and opening new possibilities for investigating high-frequency transitions.

Contribution

The authors developed a transient field-resolved reflectometry technique at 50-100 THz with MHz repetition rate and sub-10 fs resolution, expanding the frequency range of ultrafast spectroscopy.

Findings

Demonstrated the technique on Ge and GaAs semiconductors

Explored resonance-free Drude response at high frequencies

Enabled studies of intramolecular vibrations in various systems

Abstract

Transient field-resolved spectroscopy enables studies of ultrafast dynamics in molecules, nanostructures, or solids with sub-cycle resolution, but previous work has so far concentrated on extracting the dielectric response at frequencies below 50\,THz. Here, we implemented transient field-resolved reflectometry at 50-100\,THz (3-6\,$\mu$m) with MHz repetition rate employing 800\,nm few-cycle excitation pulses that provide sub-10\,fs temporal resolution. The capabilities of the technique are demonstrated in studies of ultrafast photorefractive changes in the semiconductors Ge and GaAs, where the high frequency range permitted to explore the resonance-free Drude response. The extended frequency range in transient field-resolved spectroscopy can further enable studies with so far inaccessible transitions, including intramolecular vibrations in a large range of systems.