2D-Raman-THz spectroscopy with single-shot THz detection

J Chem Phys. 2021 Nov 7;155(17):174201. doi: 10.1063/5.0065804.

Abstract

We present a 2D-Raman-terahertz (THz) setup with multichannel (single-shot) THz detection, utilizing two crossed echelons, in order to reduce the acquisition time of typical 2D-Raman-THz experiments from days to a few hours. This speed-up is obtained in combination with a high repetition rate (100 kHz) Yb-based femtosecond laser system and a correspondingly fast array detector. The wavelength of the Yb-laser (1030 nm) is advantageous, since it assures almost perfect phase matching in GaP for THz generation and detection and since the dispersion in the transmissive echelons is minimal. 2D-Raman-THz test measurements on liquid bromoform (CHBr3) are reported. An enhancement of a factor ∼5.8 in signal-to-noise ratio is obtained for single-shot detection when compared to conventional step-scanning measurements in the THz time domain, corresponding to a speed-up of acquisition time of ∼34.