Two-frequency CARS imaging by switching fiber laser excitation.

To fully exploit the power of coherent Raman imaging, techniques are needed to image more than one vibrational frequency simultaneously. We describe a method for switching between two vibrational frequencies based on a single fiber-laser source. Stokes pulses were generated by soliton self-frequency shifting in a photonic crystal fiber. Pump and Stokes pulses were stretched to enhance vibrational resolution by spectral focusing. Stokes pulses were switched between two wavelengths on the millisecond time scale by a liquid-crystal retarder. Proof-of-principle is demonstrated by coherent anti-Stokes Raman imaging of polystyrene beads embedded in a poly(methyl methacrylate) (PMMA) matrix. The Stokes shift was switched between 3,050 cm , where polystyrene has a Raman transition, and 2,950 cm , where both polystyrene and PMMA have Raman resonances. The method can be extended to multiple vibrational modes.