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The ability to enhance resonant signals and eliminate the non-resonantbackground is analyzed for Coherent Anti-Stokes Raman Scattering (CARS). Theanalysis is done at a specific frequency as well as for broadband excitationusing femtosecond pulse-shaping techniques. An appropriate objective functionalis employed to balance resonant signal enhancement against non-resonantbackground suppression. Optimal enhancement of the signal and minimization ofthe background can be achieved by shaping the probe pulse alone while keepingthe pump and Stokes pulses in transform-limited-form (TLF). In some casesanalytical forms for the probe pulse can be found, and numerical simulationsare carried out for other circumstances. It is found that a good approximatesolution for the optimal pulse in the two-pulse CARS is a superposition oflinear and arctangent type phases for the pump. The well-known probe delaymethod is shown to be a quasi-optimal scheme for background suppression. Theresults should provide a basis to improve the performance of CARS spectroscopyand microscopy.

Optimal coherent control of CARS: signal enhancement and background elimination