title: Coherently-controlled two-dimensional photon echo electronic spectroscopy.
abstract: Optical two-dimensional photon-echo spectroscopy is realized with shaped excitation pulses, allowing coherent control of twodimensional spectra. This development enables probing of state-selective quantum decoherence and phase/time sensitive couplings between states. The coherently-controlled two-dimensional photon-echo spectrometer with two pulse shapers is based on a passively stabilized four-beam interferometer with diffractive optic, and allows heterodyne detection of signals with a long-term phase stability of approximately Lambda/100. The two-dimensional spectra of Rhodamine 101 in a methanol solution, measured with unshaped and shaped pulses, exhibit significant differences. We observe in particular, the appearance of fine structure in the spectra obtained using shaped excitation pulses.
authors.affiliation: Departments of Chemistry and Physics, University of Toronto, Toronto, ON, Canada. prokh@lphys.chem.utoronto.ca
authors.forename: Valentyn I
authors.initials: VI
authors.lastname: Prokhorenko
authors.forename: Alexei
authors.initials: A
authors.lastname: Halpin
authors.forename: R J D
authors.initials: RJ
authors.lastname: Miller
mesh_terms: D017076:Computer-Aided Design; D004581:Electronics / Q000295:instrumentation*; D004867:Equipment Design; D019544:Equipment Failure Analysis; D017785:Photons; D015203:Reproducibility of Results; D012680:Sensitivity and Specificity; D013057:Spectrum Analysis / Q000295:instrumentation*; D041623:Tomography, Optical Coherence / Q000295:instrumentation*