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Coherent Raman spectro-imaging with laser frequency combs

Abstract

Advances in optical spectroscopy and microscopy have had a profound impact throughout the physical, chemical and biological sciences. One example is coherent Raman spectroscopy, a versatile technique interrogating vibrational transitions in molecules. It offers high spatial resolution and three-dimensional sectioning capabilities that make it a label-free tool1,2 for the non-destructive and chemically selective probing of complex systems. Indeed, single-colour Raman bands have been imaged in biological tissue at video rates3,4 by using ultra-short-pulse lasers. However, identifying multiple, and possibly unknown, molecules requires broad spectral bandwidth and high resolution. Moderate spectral spans combined with high-speed acquisition are now within reach using multichannel detection5 or frequency-swept laser beams6,7,8,9. Laser frequency combs10 are finding increasing use for broadband molecular linear absorption spectroscopy11,12,13,14,15. Here we show, by exploring their potential for nonlinear spectroscopy16, that they can be harnessed for coherent anti-Stokes Raman spectroscopy and spectro-imaging. The method uses two combs and can simultaneously measure, on the microsecond timescale, all spectral elements over a wide bandwidth and with high resolution on a single photodetector. Although the overall measurement time in our proof-of-principle experiments is limited by the waiting times between successive spectral acquisitions, this limitation can be overcome with further system development. We therefore expect that our approach of using laser frequency combs will not only enable new applications for nonlinear microscopy but also benefit other nonlinear spectroscopic techniques.

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Figure 1: Principle of dual-comb CARS.
Figure 2: Experimental setup for dual-comb CARS spectro-imaging.
Figure 3: High-resolution dual-comb CARS of a mixture of liquid chemicals.
Figure 4: Hyperspectral image of a capillary plate with holes filled with a chemical mixture.

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Acknowledgements

We thank P. Hommelhoff, M. Schultze and W. Schweinberger for the loan of optical components, and A. Hipke for experimental support. Research was conducted in the scope of the European Laboratory for Frequency Comb Spectroscopy. We acknowledge support from the Max Planck Foundation, the Munich Center for Advanced Photonics, Eurostars and the European Research Council (Advanced Investigator grant no. 267854).

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T.I. and S.H. contributed equally to the experimental work. All authors contributed extensively to the work presented in this paper.

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Correspondence to Nathalie Picqué.

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The authors declare no competing financial interests.

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This file contains Supplementary Text and Data 1-2, Supplementary Tables 1-3 and additional references. (PDF 304 kb)

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Ideguchi, T., Holzner, S., Bernhardt, B. et al. Coherent Raman spectro-imaging with laser frequency combs. Nature 502, 355–358 (2013). https://doi.org/10.1038/nature12607

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