title: Spectral quantum beating in mixed frequency/time-domain coherent multidimensional spectroscopy.
abstract: Coherent multidimensional spectroscopy performed in the mixed frequency/time domain exhibits both temporal and spectral quantum beating when two quantum states are simultaneously excited. The excitation of both quantum states can occur because either the spectral width of the states or the excitation pulse exceeds the frequency separation of the quantum states. The quantum beating appears as a line that broadens and splits into two peaks and then recombines as the time delay between excitation pulses increases. The splitting depends on the spectral width of the excitation pulses. We observe the spectral quantum beating between the two nearly degenerate asymmetric carbonyl stretch modes in a nickel tricarbonyl chelate using the nonrephasing, ground state bleaching coherence pathway in triply vibrationally enhanced four-wave mixing as the time delay between the first two excitation pulses changes.
authors.affiliation: Department of Chemistry, University of Wisconsin, Madison, WI 53706, USA.
authors.forename: Andrei V
authors.initials: AV
authors.lastname: Pakoulev
authors.forename: Mark A
authors.initials: MA
authors.lastname: Rickard
authors.forename: Nathan A
authors.initials: NA
authors.lastname: Mathew
authors.forename: Kathryn M
authors.initials: KM
authors.lastname: Kornau
authors.forename: John C
authors.initials: JC
authors.lastname: Wright
mesh_terms: D002614:Chelating Agents / Q000737:chemistry*; D003198:Computer Simulation; D008958:Models, Molecular; D009532:Nickel / Q000737:chemistry; D011789:Quantum Theory; D013057:Spectrum Analysis; D013997:Time Factors
chemical_list: D002614:Chelating Agents; D009532:Nickel