We demonstrate experimentally that coherent anti-Stokes Raman microspectroscopy with high spectral resolution is achieved using femtosecond laser pulses chirped up to a few picoseconds by glass elements of known group-velocity dispersion without significant intensity losses. By simply choosing the length of the glass, the chirp of Stokes and pump pulses is tailored to obtain a spectral resolution given by the Fourier limit of the chirped pulse duration. We show that for chirped pulse durations shorter than or comparable to the Raman coherence time, maximum signal occurs for a pump arriving after the Stokes pulse, a time-ordering effect confirmed by numerical simulations.

We present the implementation of a combined digital scanned light-sheet microscope (DSLM) able to work in the linear and nonlinear regimes under either Gaussian or Bessel beam excitation schemes. A complete characterization of the setup is performed and a comparison of the performance of each DSLM imaging modality is presented using in vivo Caenorhabditis elegans samples. We found that the use of Bessel beam nonlinear excitation results in better image contrast over a wider field of view.

We demonstrate coherent anti-Stokes Raman scattering (CARS) microspectroscopy using a single Ti:sapphire laser oscillator and simple passive optical elements. Spectral selection by dichroic mirrors and linear chirping by glass elements creates a vibrational excitation tuneable over a large spectral range $\left(\sim 800–2200{\text{cm}}^{-1}\right)$ with adjustable spectral resolution $\left(\sim 10–100{\text{cm}}^{-1}\right)$ . We furthermore demonstrate the applicability of differential CARS, enhancing the chemical selectivity, with the proposed single-laser configuration.

We demonstrate a technique for differential coherent anti-Stokes Raman scattering (CARS) microscopy employing linearly chirped femtosecond laser pulses. By replicating the exciting pump-Stokes pulse pairs to create a pulse train at twice the laser repetition rate, and controlling the instantaneous frequency difference of each pair by glass dispersion, we can adjust the Raman frequency probed by each pair in an intrinsically stable and cost-effective way. The resulting CARS intensities are detected by a single photomultiplier as sum and difference using phase-sensitive frequency filtering. We demonstrate imaging of polymer beads and living cells with suppressed nonresonant CARS background and improved chemical sensitivity.