title: Can stimulated Raman pumping cause large population transfers in isolated molecules?
abstract: When stimulated Raman pumping (SRP) is applied to a stream of isolated molecules, such as found in a supersonic molecular beam expansion, we show that SRP can neither saturate nor power broaden a molecular transition connecting two metastable levels that is resonant with the energy difference between the pump and Stokes laser pulses. Using the optical Bloch-Feynman equations, we discuss the pumping of the hydrogen molecule from H(2) (v = 0, J = 0, M = 0) to H(2) (v = 1, J =  2, M = 0) as an illustration of how coherent population return severely reduces the SRP pumping efficiency unless the pump and Stokes laser pulses are applied with an appropriate relative delay and ratio of intensities.
authors.affiliation: Department of Chemistry, Stanford University, Stanford, California 94305-5080, USA.
authors.forename: Nandini
authors.initials: N
authors.lastname: Mukherjee
authors.forename: Richard N
authors.initials: RN
authors.lastname: Zare