We demonstrate coherent Raman spectroscopy (CRS) using a tunable excitation source based on a single femtosecond fiber laser. The frequency difference between the pump and the Stokes pulses was generated by soliton self-frequency shifting in a nonlinear optical fiber. Spectra of stretches of cyclohexane were measured simultaneously by stimulated Raman gain (SRG) and coherent anti-Stokes Raman scattering (CARS) and compared. We demonstrate the use of spectral focusing through pulse chirping to improve CRS spectral resolution. We analyze the impact of pulse stretching on the reduction of power efficiency for CARS and SRG. Due to chromatic dispersion in the fiber-optic system, the differential pulse delay is a function of Stokes wavelength. This differential delay has to be accounted for when spectroscopy is performed in which the Stokes wavelength needs to be scanned. CARS and SRG signals were collected and displayed in two dimensions as a function of both the time delay between chirped pulses and the Stokes wavelength, and we demonstrate how to find the stimulated Raman spectrum from the two-dimensional plots. Strategies of system optimization consideration are discussed in terms of practical applications.
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