Stimulated Raman scattering holography for time-resolved imaging of methane gas

In this paper, pulsed digital holographic detection is coupled to the stimulated Raman scattering (SRS) process for imaging gases. A Q-switched Nd-YAG laser (532 nm) has been used to pump methane gas (CH₄) at pressures up to 12 bars. The frequency-tripled (355 nm) beam from the same laser was used to pump an optical parametric oscillator (OPO). The Stokes beam (from the OPO) has been tuned to 629.93 nm so that the frequency difference between the pump (532 nm) and the Stokes beams fits a Raman active vibrational mode of the methane molecule (2922  cm^-1). The pump beam has been spatially modulated with fringes produced in a Michelson interferometer. The pump and the Stokes beams were overlapped in time, space, and polarization on the gas molecules, resulting in a stimulated Raman gain of the Stokes beam and a corresponding loss of the pump beam through the SRS process. The resulting gain of the Stokes beam has been detected using pulsed digital holography by blending it with a reference beam on the detector. Two holograms of the Stokes beam, without and with the pump beam fringes present, were recorded. Intensity maps calculated from the recorded digital holograms showed amplification of the Stokes beam at the position of overlap with the pump beam fringes and the gas molecules. The gain of the Stokes beam has been separated from the background in the Fourier domain. A gain of about 4.5% at a pump beam average intensity of 4  MW/cm² and a Stokes beam intensity of 0.16  MW/cm² have been recorded at a gas pressure of 12 bars. The gain decreased linearly with decreasing gas pressure. The results show that SRS holography is a promising technique to pinpoint a specific species and record its spatial and temporal distribution.