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Preparation of a selected high vibrational energy level of isolated molecules.
Journal of Chemical Physics 2016 October 22
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 a demonstration, we transfer nearly 100 percent of the HD (v = 0, J = 0) in a supersonically expanded molecular beam of HD molecules 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. By comparing our experimental data with our theoretical calculations, we are able to draw two important conclusions: (1) using SARP a large population (>10(10) molecules per laser pulse) is prepared in the (v = 4, J = 0) level of HD and (2) the polarizability α00,40 (≅0.6 × 10(-41) C m(2) V(-1)) for the (v = 0, J = 0) to (v = 4, J = 0) Raman overtone transition is only about five times smaller than α00,10 for the (v = 0, J = 0) to (v = 1, J = 0) fundamental Raman transition. Moreover, the SARP process selects a specific rotational level in the vibrational manifold and can prepare one or a phased linear combination of magnetic sublevels (M states) within the selected vibrational-rotational level. This capability of preparing selected, highly excited vibrational levels of molecules under collision-free conditions opens new opportunities for fundamental scattering experiments.
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