Enhancing strong-field induced molecular vibration with femtosecond pulse shaping

This work investigates the utility of femtosecond pulse shaping in increasing the efficiency of Raman excitation of molecules in the strong-field interaction regime. We study experimentally and theoretically the effect of pulse shaping on the strength of non-resonant coherent anti-Stokes Raman scattering in iodine vapor at laser intensities exceeding ${10}^{13}$ W/cm${}^2$. We show that unlike the perturbative case, shaping strong non-resonant laser pulses can increase the signal strength beyond that observed with the transform-limited excitation. Both adiabatic and non-adiabatic schemes of excitation are explored, and the differences of their potential in increasing the excitation efficiency are discussed.