Stimulated Raman lineshapes in the large light-matter interaction limit

Abstract: Stimulated Raman scattering (SRS) represents a powerful tool for accessing the vibrational properties of molecular compounds or solid state systems. From a spectroscopic perspective, SRS is able to capture Raman spectra free from incoherent background processes and typically ensures a signal enhancement of several orders of magnitude with respect to its spontaneous counterpart. Since its discovery in 1962, SRS has been applied to develop technological applications, such as Raman-based lasers, frequency shifters for pulsed sources and Raman amplifiers. For the full exploitation of their potential, however, it is crucial to have an accurate description of the SRS processes under the large gain regime. Here, by taking as an example the stimulated Raman spectrum of a model solvent, namely liquid cyclohexane, we discuss how the spectral profiles and the lineshapes of Raman excitations critically depend on the pump excitation regime. In particular, we show that in the large light-matter interaction limit the Raman gain undergoes an exponential increase (decrease) in the red (blue) side of the spectrum, with the Raman linewidths that appear sharpened (broadened).