Highly Efficient Pumping of Vibrationally Excited HD Molecules via Stark-Induced Adiabatic Raman Passage

A primary prerequisite to study reactivity of vibrationally excited species is to efficiently prepare reacting species in a well-defined vibrational level. Efficient pumping of IR active vibrational modes in a molecule can be achieved by direct IR absorption. For vibrational modes that are only Raman active, however, efficient preparation of vibrationally excited states in those modes is not easily attainable. In this work, we have shown that highly efficient preparation of the HD­(v = 1) state using the Stark-induced adiabatic Raman passage (SARP) scheme is feasible. As high as 91% population transfer from v = 0 to 1 of HD has been demonstrated in our experiment. This method provides new opportunities for future experimental studies on the dynamics of vibrational state molecules, especially H₂, in both gas-phase and beam-surface reactions.