Abstract
Abstract : During the course of this ARO project we proposed [J. Chem. Phys. 135, 024201 (2011)] that using stimulated Raman adiabatic passage (SARP) with partially overlapping pump and Stokes laser pulses it is possible to transfer the complete ground state population of an isolated diatomic molecule to an excited rovibrational eigenstate. Based on this idea we carried out experiments using a sequence of overlapping pump (532 nm) and Stokes (683 nm) single-mode laser pulses of unequal fluence to prepare isolated H2 molecules in a molecular beam. In a first series of experiments we were able to transfer more than half the population of H2 (v=0, J=0) level to an excited rovibrational level [J. Chem. Phys. 138, 051101-1-4 (2013)]. Since then, we have achieved almost complete transfer (97 7%) of population from the H2 (v=0, J=0) ground rovibrational level to the H2 (v=1, J=0) excited rovibrational level [W. Dong, N. Mukherjee and R. N. Zare, J. Chem. Phys. 139, 074204 (2013)]. SARP opens new avenues to explore reaction dynamics using single or coherent superposition of quantum states.
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