Coherently-controlled two-dimensional photon echo electronic spectroscopy

Optical two-dimensional photon-echo spectroscopy is realized with shaped excitation pulses, allowing coherent control of two-dimensional 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 similar to 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. (C) 2009 Optical Society of America