Resolving molecular vibronic structure using high-sensitivity two-dimensional electronic spectroscopy

Bizimana, Laurie A.; Brazard, Johanna; Carbery, William P.; Gellen, Tobias

doi:10.1063/1.4934717

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Resolving molecular vibronic structure using high-sensitivity two-dimensional electronic spectroscopy

Bizimana, Laurie A.·Brazard, Johanna·Carbery, William P.·Gellen, Tobias

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Abstract

Coherent multidimensional optical spectroscopy is an emerging technique for resolving structure and ultrafast dynamics of molecules, proteins, semiconductors, and other materials. A current challenge is the quality of kinetics that are examined as a function of waiting time. Inspired by noise-suppression methods of transient absorption, here we incorporate shot-by-shot acquisitions and balanced detection into coherent multidimensional optical spectroscopy. We demonstrate that implementing noise-suppression methods in two-dimensional electronic spectroscopy not only improves the quality of features in individual spectra but also increases the sensitivity to ultrafast time-dependent changes in the spectral features. Measurements on cresyl violet perchlorate are consistent with the vibronic pattern predicted by theoretical models of a highly displaced harmonic oscillator. The noise-suppression methods should benefit research into coherent electronic dynamics, and they can be adapted to multidimensional spectroscopies across the infrared and ultraviolet frequency ranges.

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY ABSORPTION DETECTION FREQUENCY RANGE HARMONIC OSCILLATORS KINETICS MOLECULES PERCHLORATES PROTEINS SEMICONDUCTOR MATERIALS SENSITIVITY SPECTRA SPECTROSCOPY TIME DEPENDENCE

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Bizimana, Laurie A., Brazard, Johanna, Carbery, William P., Gellen, Tobias. 2015-10-28. Resolving molecular vibronic structure using high-sensitivity two-dimensional electronic spectroscopy. https://doi.org/10.1063/1.4934717

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