title: Preparation of a selected high vibrational energy level of isolated molecules.
abstract: 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 (>1010molecules per laser pulse) is prepared in the (v = 4, J = 0) level of HD and (2) the polarizability α00,40(≅0.6 × 10-41C m2V-1) for the (v = 0, J = 0) to (v = 4, J = 0) Raman overtone transition is only about five times smaller than α00,10for 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.
authors: Department of Chemistry, Stanford University, Stanford, California 94305-5080, USA.
authors: William E
authors: WE
authors: Perreault
authors: Department of Chemistry, Stanford University, Stanford, California 94305-5080, USA.
authors: Nandini
authors: N
authors: Mukherjee
authors: Department of Chemistry, Stanford University, Stanford, California 94305-5080, USA.
authors: Richard N
authors: RN
authors: Zare