Extracting the sample response function from experimental two-dimensional terahertz-infrared-visible spectra.

Terahertz molecular motions are often probed by high-frequency molecular oscillators in different types of non-linear vibrational spectroscopy. Recently developed two-dimensional terahertz-infrared-visible spectroscopy allows direct measuring of this coupling and, thus, obtaining site-specific terahertz vibrational spectrum. However, these data are affected by the intensity and phase of the employed laser pulses. In this work, we develop a method of extracting sample response-representing solely physical properties of a material-from experimental spectra. Using dimethyl sulfoxide as a model molecule to verify this method, we measure the coupling between C-H stretch vibration of its methyl groups and terahertz intramolecular twist and wagging modes.