Coherent multidimensional optical spectra measured using incoherent light

Daniel B. Turner, Paul C. Arpin, Scott D. McClure, Darin J. Ulness, Gregory D. Scholes

Research output: Contribution to journalArticlepeer-review

25 Scopus citations


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.

Original languageEnglish (US)
Article number2298
JournalNature communications
StatePublished - Aug 29 2013
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • General Chemistry
  • General Biochemistry, Genetics and Molecular Biology
  • General Physics and Astronomy


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