title: Wavepacket and potential reconstruction by four-wave mixing spectroscopy: preliminary application to polyatomic molecules.
abstract: We have recently shown how the excited-state wavepacket of a polyatomic molecule can be completely reconstructed from resonant coherent anti-Stokes Raman spectroscopy [Avisar and Tannor, Phys. Rev. Lett., 2011, 106, 170405]. The method assumes knowledge of the ground-state potential but not of any excited-state potential, however the latter can be computed once the excited-state wavepacket is known. The formulation applies to dissociative as well as bound excited potentials. We demonstrate the method on the Li2 molecule with its bound first excited-state as well as with a model dissociative excited state potential. Preliminary results are shown for a model two-dimensional molecular system. The calculations assume constant transition dipole moment (Condon approximation), delta-pulse excitation and a single excited-state potential, but we discuss the implications of removing these assumptions.
authors.affiliation: Department of Chemical Physics, The Weizmann Institute of Science, PO Box 26, Rehovot, 76100, Israel.
authors.forename: David
authors.initials: D
authors.lastname: Avisar
authors.forename: David J
authors.initials: DJ
authors.lastname: Tannor
mesh_terms: D008094:Lithium / Q000737:chemistry*; D011789:Quantum Theory; D013057:Spectrum Analysis
chemical_list: D008094:Lithium