Control and measurement of a non-resonant Raman wavepacket using a single ultrashort pulse

Using a single shaped femtosecond pulse, a molecular wavepacket is both tailored and monitored. Several toluene vibrational levels are excited in a controlled manner, both in amplitude and phase, through a quantum coherently controlled non-resonant Raman process. The entire coherent anti-Stokes Raman spectroscopy (CARS) process, that includes excitation and probing of the Raman-induced wavepacket, is enabled by polarization and phase shaping. We achieve a wavepacket detection sensitive to the modes relative phase and further extend the capabilities of the single-pulse CARS technique.