High Resolution Mode-Selective Excitation by Adaptive Femtosecond Pulse Shaping

High resolution mode-selective excitation in the mixture of C₆H₆ (992cm^-1) and C₆D₆ (945cm^-1) is experimentally achieved by adaptive femtosecond pulse shaping based on the genetic algorithm (GA), and second harmonic generation frequency-resolved optical gating (SHG-FROG) is adopted to characterize the original and optimal laser pulses, and its mechanism is experimentally validated by tailoring the frequency components of the pump pulses at the Fourier plane. It is indicated that two-pulse coherent mode-selective excitation of the Raman scattering mainly depends on the effective
frequency components of the pump pulse related to specific molecular vibrational mode. The experimental results have attractive potential applications in the complicated molecular system.