Stark induced adiabatic Raman passage (SARP) allows us to prepare an appreciable concentration of isolated molecules in a specific, high-lying vibrational level. The process has general applicability, and as we demonstrate by transferring nearly 100% of the HD (v=0, J=0) molecules in a supersonically expanded molecular beam to HD (v=4, J=0). This is achieved with a sequence of partially overlapping nanosecond pump (355 nm) and Stokes (680 nm) single-mode laser pulses of unequal intensities. The experimental spectral broadening with delay (Fig. 1) and saturation against Stokes power (Fig. 2) suggest that complete population transfer has been achieved from the initial HD (v=0, J=0) to the target (v=4, J=0). By comparing our experimental data with our theoretical calculations we are able to draw two important conclusions: (1) using SARP a large population (&gt;1010 molecules per laser pulse) is prepared in the (v=4, J=0) level of HD, and (2) the polarizability α00,40 (0.6 x 10-41 Cm2V-1) for the (v=0, J=0) to (v=4, J=0) Raman overtone transition is about five times smaller than α00,10 for the (v=0, J=0) to (v=1, J=0) fundamental Raman transition. In addition, SARP prepares one or a superposition of magnetic sublevels in the selected rovibrational level. This capability of preparing selected, highly excited vibrational levels of molecules under collision-free conditions opens new opportunities for fundamental scattering experiments. We would like to thank the Army Research Office for funding this work.

Preparation of a single highly vibrationally excited quantum state using Stark induced adiabatic Raman passage

253rd National Meeting (2017)

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