Paper detail

Optimal coherent control of CARS: signal enhancement and background elimination

The ability to enhance resonant signals and eliminate the non-resonant background is analyzed for Coherent Anti-Stokes Raman Scattering (CARS). The analysis is done at a specific frequency as well as for broadband excitation using femtosecond pulse-shaping techniques. An appropriate objective functional is employed to balance resonant signal enhancement against non-resonant background suppression. Optimal enhancement of the signal and minimization of the background can be achieved by shaping the probe pulse alone while keeping the pump and Stokes pulses in transform-limited-form (TLF). In some cases analytical forms for the probe pulse can be found, and numerical simulations are carried out for other circumstances. It is found that a good approximate solution for the optimal pulse in the two-pulse CARS is a superposition of linear and arctangent type phases for the pump. The well-known probe delay method is shown to be a quasi-optimal scheme for background suppression. The results should provide a basis to improve the performance of CARS spectroscopy and microscopy.