Abstract

Mid-infrared ultrafast laser technologies have enabled multi-quantum vibrational excitation of molecules, and have opened a way to control molecular reactions at electronic ground states. Molecular dissociation mediated by vibrational excitation has been achieved, but subjects of application are limited to typical molecules such as W(CO)₆ and CH₂N₂ [2,3]. To realize control of molecular reactions with a high degree of freedom, such as association reactions where the orientation of the molecules affects the reaction probability, it is important to control the rotational states as well as vibrational states. In this study, we report on successful demonstration of multi-quantum vibrational excitation in the anti-symmetric stretch (ν₃) of gas-phase CO₂ molecules up to the ν₃ = 8 state and observation of the rotational wave packet in the ν₃ = 0 to 8 states.

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