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Coherent multidimensional optical spectra measured using incoherent light

Author(s): Turner, Daniel B.; Turner, Daniel B.; Turner, Daniel B.; Turner, Daniel B.; Turner, Daniel B.; et al

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Abstract: Four-wave mixing measurements can reveal spectral and dynamics information that is hidden in linear spectra by the interactions among light-absorbing molecules and with their environment. Coherent multidimensional optical spectroscopy is an important variant of four-wave mixing because it resolves a map of interactions and correlations between absorption bands. Previous coherent multidimensional optical spectroscopy measurements have used femtosecond pulses with great success, and it may seem that femtosecond pulses are necessary for such measurements. Here we present coherent two-dimensional electronic spectra measured using incoherent light. The spectra of model molecular systems using broadband spectrally incoherent light are similar but not identical to those expected from measurements using femtosecond pulses. Specifically, the spectra show particular sensitivity to long-lived intermediates such as photoisomers. The results will motivate the design of similar experiments in spectral ranges where femtosecond pulses are difficult to produce. © 2013 Macmillan Publishers Limited. All rights reserved.
Publication Date: 29-Aug-2013
Citation: Turner, Daniel B., Arpin, Paul C., McClure, Scott D., Ulness, Darin J., Scholes, Gregory D. (2013). Coherent multidimensional optical spectra measured using incoherent light. Nature Communications, 4 (1), 10.1038/ncomms3298
DOI: doi:10.1038/ncomms3298
EISSN: 2041-1723
Pages: 4.29:2298-1 - 2298-9
Type of Material: Journal Article
Journal/Proceeding Title: Nature Communications
Version: Final published version. This is an open access article.
Notes: Nature Communications. Volume 4, 29 August 2013, Article number 2298.

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