With the present paper, we demonstrate an experimental setup connecting two highly innovative fields of research: stimulated Raman scattering (SRS) spectroscopy and terahertz (THz) spectroscopy of liquids. For this purpose, we use the spectral focusing method allowing us to excite and measure molecular vibrations by chirped laser pulses. With our experimental setup, we apply this method to the THz regime in order to detect the frequency dependence of SRS processes in organic liquids. More specifically, we focus two chirped laser pulses onto the sample to drive molecular vibrations at THz frequencies. Thereby, the time delay between the laser pulses is directly related to the driving frequency. Due to SRS process, an energy transfer between the two laser pulses is established. By detecting the corresponding energy change of only one of the two laser pulses, we are able to observe inverse Raman scattering and stimulated Raman gain scattering as well as the transition between both processes at zero delay time. The peak positions and the line shapes of the measured spectra agree well with literature data obtained by spontaneous Raman scattering spectroscopy and optical heterodyne detection optical Kerr effect spectroscopy. With the present setup, we are able to excite and detect molecular vibrations ranging over two orders of magnitude from 10 THz to ultra-low frequencies at 100 GHz.
References
As as stimulated Raman scattering, we summarize inverse Raman scattering (also denoted by the literature as stimulated Raman loss scattering) and stimulated Raman gain scattering.
