Dissection of rovibronic structure by polarization-resolved two-color resonant four-wave mixing spectroscopy.

摘要: A synergistic theoretical and experimental investigation of stimulated emission pumping (SEP) as implemented in the coherent framework two-color resonant four-wave mixing (TC-RFWM) spectroscopy is presented, with special emphasis directed toward identification polarization geometries that can distinguish spectral features according to their attendant changes rotational quantum numbers. vector-recoupling formalism built upon a perturbative treatment matter-field interactions state-multipole expansion density operator allowed weak-field signal intensity be cast terms TC-RFWM response tensor, RQ(K)(e4*e3e2*e1;Jg,Je,Jh,Jf), which separates transverse characteristics incident generated electromagnetic waves (e4*e3e2*e1) from angular momentum properties PUMP DUMP resonances (Jg,Je,Jh,Jf). For an isolated SEP process induced isotropic medium, criteria needed discriminate against subsets rovibronic structure were encoded i...