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Coherent multidimensional optical spectra measured using incoherent light

Author

Listed:
  • Daniel B. Turner

    (Institute for Optical Sciences and Centre for Quantum Information and Quantum Control, University of Toronto)

  • Paul C. Arpin

    (Institute for Optical Sciences and Centre for Quantum Information and Quantum Control, University of Toronto)

  • Scott D. McClure

    (Institute for Optical Sciences and Centre for Quantum Information and Quantum Control, University of Toronto)

  • Darin J. Ulness

    (Concordia College)

  • Gregory D. Scholes

    (Institute for Optical Sciences and Centre for Quantum Information and Quantum Control, University of Toronto)

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.

Suggested Citation

  • Daniel B. Turner & Paul C. Arpin & Scott D. McClure & Darin J. Ulness & Gregory D. Scholes, 2013. "Coherent multidimensional optical spectra measured using incoherent light," Nature Communications, Nature, vol. 4(1), pages 1-9, October.
    • Handle: RePEc:nat:natcom:v:4:y:2013:i:1:d:10.1038_ncomms3298
    DOI: 10.1038/ncomms3298
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    Cited by:

    1. Magnus Röding & Siobhan J Bradley & Nathan H Williamson & Melissa R Dewi & Thomas Nann & Magnus Nydén, 2016. "The Power of Heterogeneity: Parameter Relationships from Distributions," PLOS ONE, Public Library of Science, vol. 11(5), pages 1-11, May.

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