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Coherent Raman spectro-imaging with laser frequency combs
Open accessAbstract
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 tool for the non-destructive and chemically selective probing of complex systems. Indeed, single-colour Raman bands have been imaged in biological tissue at video rates 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 detection or frequency-swept laser beams. Laser frequency combs are finding increasing use for broadband molecular linear absorption spectroscopy. Here we show, by exploring their potential for nonlinear spectroscopy, 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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Citations
Cites
Principles of Nonlinear Optical Spectroscopy
Mukamel, S. (1995) · Cited by 4,640
Microresonator-Based Optical Frequency Combs
Kippenberg, T. J., Holzwarth, R., & Diddams, S. A. (2011) · Science · doi:10.1126/science.1193968 · Cited by 2,159
Schließer, A., Picqué, N., & Hänsch, T. W. (2012) · Nature Photonics · doi:10.1038/nphoton.2012.142 · Cited by 1,468
Self-citationChemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy
Evans, C. L., Potma, E. O., Puoris'haag, M., Côté, D., Lin, C. P., & Xie, X. S. (2005) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.0508282102 · Cited by 957
Nobel Lecture: Passion for precision
Hänsch, T. W. (2006) · Reviews of Modern Physics · doi:10.1103/revmodphys.78.1297 · Cited by 913
Self-citationVideo-Rate Molecular Imaging in Vivo with Stimulated Raman Scattering
Saar, B. G., Freudiger, C. W., Reichman, J. R., Stanley, C. M., Holtom, G. R., & Xie, X. S. (2010) · Science · doi:10.1126/science.1197236 · Cited by 838
Coherent Multiheterodyne Spectroscopy Using Stabilized Optical Frequency Combs
Coddington, I. R., Swann, W. C., & Newbury, N. R. (2008) · Physical Review Letters · doi:10.1103/physrevlett.100.013902 · Cited by 821
Molecular fingerprinting with the resolved modes of a femtosecond laser frequency comb
Diddams, S. A., Hollberg, L. W., & Mbele, V. (2007) · Nature · doi:10.1038/nature05524 · Cited by 799
Serial time-encoded amplified imaging for real-time observation of fast dynamic phenomena
Goda, K., Tsia, K., & Jalali, B. (2009) · Nature · doi:10.1038/nature07980 · Cited by 753
Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy
Dudovich, N., Oron, D., & Silberberg, Y. R. (2002) · Nature · doi:10.1038/nature00933 · Cited by 732
Flagged first, then by citations
1 of the 39 references couldn’t be matched to a known paper.
Research works printed but not linked: 2
- Cheng J. X., Xie X. S., eds. Coherent Raman Scattering Microscopy (CRC Press, 2012)
- Boyd, R. W. Nonlinear Optics 3rd edn, Ch. 10.3 (Academic, 2008)
Cited by
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Items 401–475 of 475
Yoon, W., Choi, Y., Kang, D., Bang, K.-C., & Jeong, K. (2018) · Proceedings of the World Congress on Recent Advances in Nanotechnology · doi:10.11159/icnnfc18.126
Use of Lock-in Detection in Dual-Comb Spectroscopy
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Nürnberg, J., Alfieri, C. G. E., Waldburger, D., Golling, M., & Keller, U. (2019) · Vertical External Cavity Surface Emitting Lasers (VECSELs) · doi:10.1117/12.2513209
Combination of Lock-in Detection with Dual-Comb Spectroscopy
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Sinjab, F., Hashimoto, K., Badarla, V. R., Nagashima, Y., & Ideguchi, T. (2019) · Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC) · doi:10.1109/cleoe-eqec.2019.8872300
Self-citationHan, N. S., Kim, J., Yoon, T. H., & Cho, M. (2020) · arXiv (Cornell University) · doi:10.48550/arxiv.2001.05179
6-octave UV to MIR frequency comb driven by a <10 fs Er:fiber laser
Lesko, D., Timmers, H. R., Xing, S., Kowligy, A. S., Lind, A. J., Zawilski, K. T., Schunemann, P. G., & Diddams, S. A. (2020) · Conference on Lasers and Electro-Optics · doi:10.1364/cleo_si.2020.sw4n.7
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Voumard, T., Wildi, T., Brasch, V., Gutierrez-Alvarez, R., Vergara, G., & Herr, T. (2020) · Conference on Lasers and Electro-Optics · doi:10.1364/cleo_si.2020.sth3f.4
Minoshima, K. (2018) · The Review of Laser Engineering · doi:10.2184/lsj.46.7_356
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Picqué, N. (2020) · Frontiers in Optics · doi:10.1364/ls.2020.ltu4a.1
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Picqué, N. (2021) · OSA Optical Sensors and Sensing Congress 2021 (AIS, FTS, HISE, SENSORS, ES) · doi:10.1364/es.2021.eth2a.1
Self-citationYang, H., Zhang, S., Yang, W., Zhao, H., Dong, M., Jiao, W., & Ge, J. (2021) · IEEE Optoelectronics Global Conference (OGC) · doi:10.1109/ogc52961.2021.9654288
Vasa, P. R., & Mathur, D. (2016) · Biological and medical physics, biomedical engineering · doi:10.1007/978-3-319-39614-9_11
Attenuated Total Reflectance Dual-Comb Spectroscopy of an Organic Liquid-Phase Chemical Reaction
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Koresawa, H., Shibuya, K., Minamikawa, T., Asahara, A., Minoshima, K., & Yasui, T. (2019) · Photonic Instrumentation Engineering · doi:10.1117/12.2509619
Fourier transform spectroscopy with laser frequency combs
Picqué, N. (2015) · Fourier Transform Spectroscopy/ Hyperspectral Imaging and Sounding of the Environment · doi:10.1364/fts.2015.ft2a.1
Self-citationDual-Comb Digital Holography at Fast Sampling Rate
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Flöry, T., Stummer, V., Pupeikis, J., Willenberg, B., Phillips, C. R., Keller, U., Pugzlys, A., & Baltuška, A. (2022) · International Conference on Ultrafast Phenomena · doi:10.1364/up.2022.th2a.5
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Ochoa, H. G., Ramírez-Meléndez, G., Hernandez, J., & Gómez, E. (2026) · Journal of Optics · doi:10.1088/2040-8986/ae5fa6
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Metadata
- Authors
- Ideguchi, T., Holzner, S., Bernhardt, B., Guelachvili, G., Picqué, N., & Hänsch, T. W.
- Affiliations
- Max Planck Institute of Quantum Optics (DE)
- Université Paris-Sud (FR)
- Corresponding author
- Picqué, Nathalie
- Venue
- Nature
- Published
- 2013-10-16
- Volume
- 502
- Issue
- 7471
- Pages
- 355-358
- ISSN
- 0028-0836 (ISSN-L)
- 1476-4687
- OpenAlex
- W2074049639
- Cited by
- 475
- References
- 39
- Citations by year
- 2026: 16 · 2025: 30 · 2024: 38 · 2023: 47 · 2022: 33 · 2021: 35 · 2020: 38 · 2019: 43 · 2018: 44 · 2017: 48 · 2016: 38 · 2015: 34 · 2014: 26 · 2013: 5
- FWCI
- 20.81
- Type
- journal article
- Language
- en
- Open access
- green
- arxiv.org
- Locations
- Nature (publishedVersion)
- PubMed (publishedVersion)
- arXiv (Cornell University) (submittedVersion)
- RePEc: Research Papers in Economics (submittedVersion)
- MPG.PuRe (Max Planck Society) (submittedVersion)
- arXiv (Cornell University)
- Topics
- Life Sciences › Biochemistry, Genetics and Molecular Biology › Biophysics › Spectroscopy Techniques in Biomedical and Chemical Research
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
- Physical Sciences › Chemistry › Spectroscopy › Spectroscopy and Laser Applications
- Keywords
- coherent anti-Stokes Raman spectroscopy, laser frequency combs, label-free molecular imaging, nonlinear optical microscopy
- MeSH terms
- Lasers, Spectrum Analysis, Raman, Time Factors, Vibration
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