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Tri-comb spectroscopy

Nature Photonicsvolume 12pages676680 (2018) | Download Citation


Multidimensional coherent spectroscopy (MDCS)1,2 is a powerful method that enables the measurement of homogeneous linewidths in inhomogenously broadened systems, many-body interactions and coupling between excited resonances, all of which are not simultaneously accessible by any other method. Current implementations of MDCS require a bulky apparatus and suffer from resolution and acquisition speed limitations that constrain their applications outside the laboratory3,4,5. Here, we propose and demonstrate an approach to nonlinear coherent spectroscopy that utilizes three slightly different repetition-rate frequency combs. Unlike traditional nonlinear methods, tri-comb spectroscopy uses only a single photodetector and no mechanical moving elements to enable faster acquisition times, while also providing comb resolution. As a proof of concept, a multidimensional coherent spectrum with comb cross-diagonal resolution is generated using only 365 ms of data. These improvements make MDCS relevant for systems with narrow resonances and it has the potential to be field deployable for chemical-sensing applications.

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  1. 1.

    Cundiff, S. T. Coherent spectroscopy of semiconductors. Opt. Express 16, 4639–4664 (2008).

  2. 2.

    Hamm, P. & Zanni, M. Concepts and Methods of 2D Infrared Spectroscopy (Cambridge Univ. Press, New York, 2011).

  3. 3.

    Draeger, S., Roeding, S. & Brixner, T. Rapid-scan coherent 2D fluorescence spectroscopy. Opt. Express 25, 3259–3267 (2017).

  4. 4.

    Fuller, F. D., Wilcox, D. E. & Ogilvie, J. P. Pulse shaping based two-dimensional electronic spectroscopy in a background free geometry. Opt. Express 22, 1018–1027 (2014).

  5. 5.

    Harel, E., Fidler, A. F. & Engel, G. S. Real-time mapping of electronic structure with single-shot two-dimensional electronic spectroscopy. Proc. Natl Acad. Sci. USA 107, 16444–16447 (2010).

  6. 6.

    Coddington, I., Newbury, N. & Swann, W. Dual-comb spectroscopy. Optica 3, 414–426 (2016).

  7. 7.

    Coddington, I., Swann, W. C. & Newbury, N. R. Coherent multiheterodyne spectroscopy using stabilized optical frequency combs. Phys. Rev. Lett. 100, 013902 (2008).

  8. 8.

    Kippenberg, T. J., Holzwarth, R. & Diddams, S. A. Microresonator-based optical frequency combs. Science 332, 555–559 (2011).

  9. 9.

    Suh, M.-G., Yang, Q.-F., Yang, K. Y., Yi, X. & Vahala, K. J. Microresonator soliton dual-comb spectroscopy. Science 354, 600–603 (2016).

  10. 10.

    Yu, M. et al. Silicon-chip-based mid-infrared dual-comb spectroscopy. Nat. Commun. 9, 1869 (2018).

  11. 11.

    Baumann, E. et al. Spectroscopy of the methane with an accurate midinfrared coherent dual-comb spectrometer. Phys. Rev. A 84, 062513 (2011).

  12. 12.

    Bernhardt, B. et al. Cavity-enhanced dual-comb spectroscopy. Nat. Photon. 4, 55–57 (2010).

  13. 13.

    Boudreau, S., Levasseur, S., Perilla, C., Roy, S. & Genest, J. Chemical detection with hyperspectral lidar using dual frequency combs. Opt. Express 21, 7411–7418 (2013).

  14. 14.

    Brehm, M., Schliesser, A. & Keilmann, F. Spectroscopic near-field microscopy using frequency combs in the mid-infrared. Opt. Express 14, 11222–11233 (2006).

  15. 15.

    Trocha, P. et al. Ultrafast optical ranging using microresonator soliton frequency combs. Science 359, 887–891 (2018).

  16. 16.

    Suh, M.-G. & Vahala, K. J. Soliton microcomb range measurement. Science 359, 884–887 (2018).

  17. 17.

    Lomsadze, B. & Cundiff, S. T. Frequency combs enable rapid and high-resolution multidimensional coherent spectroscopy. Science 357, 1389–1391 (2017).

  18. 18.

    Cundiff, S. T. Optical two-dimensional Fourier transform spectroscopy of semiconductor nanostructures [Invited]. J. Opt. Soc. Am. B 29, A69–A81 (2012).

  19. 19.

    Kurnit, N. A., Abella, I. D. & Hartmann, S. R. Observation of a photon echo. Phys. Rev. Lett. 13, 567–568 (1964).

  20. 20.

    Boyd, R. W. Nonlinear Optics 3rd edn (Academic Press, New York, 2008).

  21. 21.

    Tekavec, P. F., Lott, G. A. & Marcus, A. H. Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation. J. Chem. Phys. 127, 214307 (2007).

  22. 22.

    Lomsadze, B. & Cundiff, S. T. Multi-heterodyne two dimensional coherent spectroscopy using frequency combs. Sci. Rep. 7, 14018 (2017).

  23. 23.

    Asahara, A. & Minoshima, K. Development of ultrafast time-resolved dual-comb spectroscopy. APL Photon. 2, 041301 (2017).

  24. 24.

    Lomsadze, B. & Cundiff, S. T. Frequency-comb based double-quantum two-dimensional spectrum identifies collective hyperfine resonances in atomic vapor induced by dipole–dipole interactions. Phys. Rev. Lett. 120, 233401 (2018).

  25. 25.

    Lomsadze, B. & Cundiff, S. T. Frequency comb-based four-wave-mixing spectroscopy. Opt. Lett. 42, 2346–2349 (2017).

  26. 26.

    Siemens, M. E., Moody, G., Li, H., Bristow, A. D. & Cundiff, S. T. Resonance lineshapes in two-dimensional Fourier transform spectroscopy. Opt. Express 18, 17699–17708 (2010).

  27. 27.

    Sinclair, L. C. et al. Invited article: a compact optically coherent fiber frequency comb. Rev. Sci. Instrum. 86, 081301 (2015).

  28. 28.

    Zhao, X. et al. Dead-band-free, high-resolution microwave frequency measurement using a free-running triple-comb fiber laser. IEEE J. Sel. Top. Quantum Electron. 24, 1–8 (2018).

  29. 29.

    Lucas, E. et al. Spatial multiplexing of soliton microcombs. Nat. Photon. https://doi.org/10.1038/s41566-018-0256-7 (2018).

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The research is based on work supported by the Office of the Director of National Intelligence (ODNI), Intelligence Advanced Research Projects Activity (IARPA), via contract 2018-18020600001. The views and conclusions contained herein are those of the authors and should not be interpreted as necessarily representing the official policies or endorsements, either expressed or implied, of the ODNI, IARPA or the US government. B.C.S. acknowledges support by the National Science Foundation through a Graduate Research Fellowship (1256260).

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    • Bachana Lomsadze

    Present address: Department of Physics, Santa Clara University, Santa Clara, CA, USA


  1. Department of Physics, University of Michigan, Ann Arbor, MI, USA

    • Bachana Lomsadze
    • , Brad C. Smith
    •  & Steven T. Cundiff


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B.L. and S.T.C. conceived the concept. B.L. and B.C.S. ran the experiment and took the data. B.L. analysed the results and wrote the manuscript. All authors discussed the results and commented on the manuscript at all stages.

Competing interests

B.L. and S.T.C. are coinventors on patent application 15/705511 submitted by the University of Michigan that covers ‘Frequency comb-based multidimensional coherent spectroscopy’.

Corresponding author

Correspondence to Steven T. Cundiff.

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