Single-beam spectrally controlled two-dimensional Raman spectroscopy


Vibrational modes are often localized in certain regions of a molecule, and so the coupling between these modes is sensitive to the molecular structure. Two-dimensional vibrational spectroscopy can probe the strength of this coupling in a manner analogous to two-dimensional NMR spectroscopy, but on ultrafast timescales. Here, we demonstrate how two-dimensional Raman spectroscopy, based on fifth-order optical nonlinearity, can be performed with a single beam of shaped femtosecond optical pulses. Our spectroscopy scheme offers not only a major simplification of the conventional set-up, but also an inherent elimination of a competing nonlinear signal, which overwhelms the desired signal in other schemes and carries no coupling information.

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Figure 1: Two-dimensional Raman spectroscopy: principle and single-beam implementation.
Figure 2: One-dimensional single-beam spectrally controlled stimulated Raman spectroscopy: experimental results.
Figure 3: Spectral control and spectrally-resolved detection of the fifth-order Raman process.
Figure 4: Two-dimensional single-beam spectrally controlled Raman spectroscopy: experimental results.
Figure 5: Comparison of the two signal-processing methods used to extract cross-peak information.


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The authors thank B. Bruner and L. Chuntonov for useful discussions. This work was supported by Icore (Israeli centres of research excellence of the ISF), the Crown Photonics Center, the Wolfson Foundation and the European ICT project FAMOS.

Author information




H.F., T.B., N.D. and Y.S. designed the experiment, analysed the data and prepared the manuscript. H.F. and T.B. performed the experiment. Y.C.E. guided the BOMP analysis.

Corresponding author

Correspondence to Yaron Silberberg.

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The authors declare no competing financial interests.

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Frostig, H., Bayer, T., Dudovich, N. et al. Single-beam spectrally controlled two-dimensional Raman spectroscopy. Nature Photon 9, 339–343 (2015).

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