Two-dimensional fluorescence-detected coherent spectroscopy with absolute phasing by confocal imaging of a dynamic grating and 27-step phase-cycling.

J Chem Phys

Physical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94702, USA.

Published: May 2014

We present a novel experimental scheme for two-dimensional fluorescence-detected coherent spectroscopy (2D-FDCS) using a non-collinear beam geometry with the aid of "confocal imaging" of dynamic (population) grating and 27-step phase-cycling to extract the signal. This arrangement obviates the need for distinct experimental designs for previously developed transmission detected non-collinear two-dimensional coherent spectroscopy (2D-CS) and collinear 2D-FDCS. We also describe a novel method for absolute phasing of the 2D spectrum. We apply this method to record 2D spectra of a fluorescent dye in solution at room temperature and observe "spectral diffusion."

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http://dx.doi.org/10.1063/1.4874697DOI Listing

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