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Chemical Physics Letters

Two-dimensional spectroscopy using diffractive optics based phased-locked photon echoes

M. L. Cowan, Jennifer P. Ogilvie, R. J. Dwayne Miller

Published Feb 10, 2004• 336 citations
Publisher
DOI
10.1016/j.cplett.2004.01.027

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•Jan 1, 2005•0 citations
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.
Nonlinear optical techniques are widely used to study energy transport in nanoscale objects. In particular photon echo spectroscopy can be used to determine if the energy transport is coherent or not. In this project a novel phase sensitive nonlinear technique is proposed. The main feature of this technique is the application of two phase-locked pulses. The relative phase and the delay between the two pulses is set electronically by a pulse shaper based on a spatial light modulator (SLM). The use of an SLM ensures phase stability. The proposed method is tested on a model system of solutions of the dye molecule DTTCI in ethylene glycol and acetonitrile. The obtained results demonstrated that the parameters from the experimental data agree with those from previous studies. Hence, the proposed technique can be further developed for energy transport studies.