Abstract

We report on the first (to our knowledge) demonstration of nonlinear dual-frequency-comb spectroscopy. In multi-heterodyne femtosecond Raman-induced Kerr-effect spectroscopy, the Raman gain resulting from the coherent excitation of molecular vibrations by a spectrally narrow pump is imprinted onto the femtosecond laser frequency comb probe spectrum. The birefringence signal induced by the nonlinear interaction of these beams and the sample is heterodyned against a frequency comb local oscillator with a repetition frequency slightly different from that of the comb probe. Such time-domain interference provides multiplex access to the phase and amplitude Raman spectra over a broad spectral bandwidth within a short measurement time.

© 2012 Optical Society of America

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  1. T. W. Hänsch, Rev. Mod. Phys. 78, 1297 (2006).
    [CrossRef]
  2. E. Baumann, F. R. Giorgetta, W. C. Swann, A. M. Zolot, I. Coddington, and N. R. Newbury, Phys. Rev. A 84, 062513 (2011).
    [CrossRef]
  3. T. Ideguchi, A. Poisson, G. Guelachvili, N. Picqué, and T. W. Hänsch, “Adaptive real-time dual-comb spectroscopy,” arXiv:1201.4177 (2012).
  4. B. Bernhardt, A. Ozawa, P. Jacquet, M. Jacquey, Y. Kobayashi, T. Udem, R. Holzwarth, G. Guelachvili, T. W. Hänsch, and N. Picqué, Nat. Photonics 4, 55 (2010).
    [CrossRef]
  5. B. Bernhardt, E. Sorokin, P. Jacquet, R. Thon, T. Becker, I. T. Sorokina, N. Picqué, and T. W. Hänsch, Appl. Phys. B 100, 3 (2010).
    [CrossRef]
  6. I. Coddington, W. C. Swann, and N. R. Newbury, Phys. Rev. Lett. 100, 013902 (2008).
    [CrossRef]
  7. A. Schliesser, N. Picqué, and T. W. Hänsch, Nat. Photonics 6, 440 (2012).
    [CrossRef]
  8. S. Shim and R. A. Mathies, J. Raman Spectrosc. 39, 1526 (2008).
    [CrossRef]
  9. D. J. Jones, E. O. Potma, J. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, Rev. Sci. Instrum. 73, 2843 (2002).
    [CrossRef]
  10. C. W. Freudiger, M. B. J. Roeffaers, X. Zhang, B. G. Saar, W. Min, and X. S. Xie, J. Phys. Chem. B 115, 5574 (2011).
    [CrossRef]
  11. C. W. Freudiger, W. Min, G. R. Holtom, B. Xu, M. Dantus, and X. S. Xie, Nat. Photonics 5, 103 (2011).
    [CrossRef]
  12. E. Ploetz, B. Marx, T. Klein, R. Huber, and P. Gilch, Opt. Express 17, 18612 (2009).
    [CrossRef]
  13. C. Wang, T. Herr, P. Del’Haye, A. Schliesser, R. Holzwarth, T. W. Hänsch, N. Picqué, and T. J. Kippenberg, “Mid-infrared frequency combs based on crystalline microresonators,” arXiv:1109.2716 (2011).

2012 (1)

A. Schliesser, N. Picqué, and T. W. Hänsch, Nat. Photonics 6, 440 (2012).
[CrossRef]

2011 (3)

C. W. Freudiger, M. B. J. Roeffaers, X. Zhang, B. G. Saar, W. Min, and X. S. Xie, J. Phys. Chem. B 115, 5574 (2011).
[CrossRef]

C. W. Freudiger, W. Min, G. R. Holtom, B. Xu, M. Dantus, and X. S. Xie, Nat. Photonics 5, 103 (2011).
[CrossRef]

E. Baumann, F. R. Giorgetta, W. C. Swann, A. M. Zolot, I. Coddington, and N. R. Newbury, Phys. Rev. A 84, 062513 (2011).
[CrossRef]

2010 (2)

B. Bernhardt, A. Ozawa, P. Jacquet, M. Jacquey, Y. Kobayashi, T. Udem, R. Holzwarth, G. Guelachvili, T. W. Hänsch, and N. Picqué, Nat. Photonics 4, 55 (2010).
[CrossRef]

B. Bernhardt, E. Sorokin, P. Jacquet, R. Thon, T. Becker, I. T. Sorokina, N. Picqué, and T. W. Hänsch, Appl. Phys. B 100, 3 (2010).
[CrossRef]

2009 (1)

2008 (2)

S. Shim and R. A. Mathies, J. Raman Spectrosc. 39, 1526 (2008).
[CrossRef]

I. Coddington, W. C. Swann, and N. R. Newbury, Phys. Rev. Lett. 100, 013902 (2008).
[CrossRef]

2006 (1)

T. W. Hänsch, Rev. Mod. Phys. 78, 1297 (2006).
[CrossRef]

2002 (1)

D. J. Jones, E. O. Potma, J. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, Rev. Sci. Instrum. 73, 2843 (2002).
[CrossRef]

Baumann, E.

E. Baumann, F. R. Giorgetta, W. C. Swann, A. M. Zolot, I. Coddington, and N. R. Newbury, Phys. Rev. A 84, 062513 (2011).
[CrossRef]

Becker, T.

B. Bernhardt, E. Sorokin, P. Jacquet, R. Thon, T. Becker, I. T. Sorokina, N. Picqué, and T. W. Hänsch, Appl. Phys. B 100, 3 (2010).
[CrossRef]

Bernhardt, B.

B. Bernhardt, E. Sorokin, P. Jacquet, R. Thon, T. Becker, I. T. Sorokina, N. Picqué, and T. W. Hänsch, Appl. Phys. B 100, 3 (2010).
[CrossRef]

B. Bernhardt, A. Ozawa, P. Jacquet, M. Jacquey, Y. Kobayashi, T. Udem, R. Holzwarth, G. Guelachvili, T. W. Hänsch, and N. Picqué, Nat. Photonics 4, 55 (2010).
[CrossRef]

Burfeindt, B.

D. J. Jones, E. O. Potma, J. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, Rev. Sci. Instrum. 73, 2843 (2002).
[CrossRef]

Cheng, J.

D. J. Jones, E. O. Potma, J. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, Rev. Sci. Instrum. 73, 2843 (2002).
[CrossRef]

Coddington, I.

E. Baumann, F. R. Giorgetta, W. C. Swann, A. M. Zolot, I. Coddington, and N. R. Newbury, Phys. Rev. A 84, 062513 (2011).
[CrossRef]

I. Coddington, W. C. Swann, and N. R. Newbury, Phys. Rev. Lett. 100, 013902 (2008).
[CrossRef]

Dantus, M.

C. W. Freudiger, W. Min, G. R. Holtom, B. Xu, M. Dantus, and X. S. Xie, Nat. Photonics 5, 103 (2011).
[CrossRef]

Del’Haye, P.

C. Wang, T. Herr, P. Del’Haye, A. Schliesser, R. Holzwarth, T. W. Hänsch, N. Picqué, and T. J. Kippenberg, “Mid-infrared frequency combs based on crystalline microresonators,” arXiv:1109.2716 (2011).

Freudiger, C. W.

C. W. Freudiger, M. B. J. Roeffaers, X. Zhang, B. G. Saar, W. Min, and X. S. Xie, J. Phys. Chem. B 115, 5574 (2011).
[CrossRef]

C. W. Freudiger, W. Min, G. R. Holtom, B. Xu, M. Dantus, and X. S. Xie, Nat. Photonics 5, 103 (2011).
[CrossRef]

Gilch, P.

Giorgetta, F. R.

E. Baumann, F. R. Giorgetta, W. C. Swann, A. M. Zolot, I. Coddington, and N. R. Newbury, Phys. Rev. A 84, 062513 (2011).
[CrossRef]

Guelachvili, G.

B. Bernhardt, A. Ozawa, P. Jacquet, M. Jacquey, Y. Kobayashi, T. Udem, R. Holzwarth, G. Guelachvili, T. W. Hänsch, and N. Picqué, Nat. Photonics 4, 55 (2010).
[CrossRef]

T. Ideguchi, A. Poisson, G. Guelachvili, N. Picqué, and T. W. Hänsch, “Adaptive real-time dual-comb spectroscopy,” arXiv:1201.4177 (2012).

Hänsch, T. W.

A. Schliesser, N. Picqué, and T. W. Hänsch, Nat. Photonics 6, 440 (2012).
[CrossRef]

B. Bernhardt, E. Sorokin, P. Jacquet, R. Thon, T. Becker, I. T. Sorokina, N. Picqué, and T. W. Hänsch, Appl. Phys. B 100, 3 (2010).
[CrossRef]

B. Bernhardt, A. Ozawa, P. Jacquet, M. Jacquey, Y. Kobayashi, T. Udem, R. Holzwarth, G. Guelachvili, T. W. Hänsch, and N. Picqué, Nat. Photonics 4, 55 (2010).
[CrossRef]

T. W. Hänsch, Rev. Mod. Phys. 78, 1297 (2006).
[CrossRef]

T. Ideguchi, A. Poisson, G. Guelachvili, N. Picqué, and T. W. Hänsch, “Adaptive real-time dual-comb spectroscopy,” arXiv:1201.4177 (2012).

C. Wang, T. Herr, P. Del’Haye, A. Schliesser, R. Holzwarth, T. W. Hänsch, N. Picqué, and T. J. Kippenberg, “Mid-infrared frequency combs based on crystalline microresonators,” arXiv:1109.2716 (2011).

Herr, T.

C. Wang, T. Herr, P. Del’Haye, A. Schliesser, R. Holzwarth, T. W. Hänsch, N. Picqué, and T. J. Kippenberg, “Mid-infrared frequency combs based on crystalline microresonators,” arXiv:1109.2716 (2011).

Holtom, G. R.

C. W. Freudiger, W. Min, G. R. Holtom, B. Xu, M. Dantus, and X. S. Xie, Nat. Photonics 5, 103 (2011).
[CrossRef]

Holzwarth, R.

B. Bernhardt, A. Ozawa, P. Jacquet, M. Jacquey, Y. Kobayashi, T. Udem, R. Holzwarth, G. Guelachvili, T. W. Hänsch, and N. Picqué, Nat. Photonics 4, 55 (2010).
[CrossRef]

C. Wang, T. Herr, P. Del’Haye, A. Schliesser, R. Holzwarth, T. W. Hänsch, N. Picqué, and T. J. Kippenberg, “Mid-infrared frequency combs based on crystalline microresonators,” arXiv:1109.2716 (2011).

Huber, R.

Ideguchi, T.

T. Ideguchi, A. Poisson, G. Guelachvili, N. Picqué, and T. W. Hänsch, “Adaptive real-time dual-comb spectroscopy,” arXiv:1201.4177 (2012).

Jacquet, P.

B. Bernhardt, E. Sorokin, P. Jacquet, R. Thon, T. Becker, I. T. Sorokina, N. Picqué, and T. W. Hänsch, Appl. Phys. B 100, 3 (2010).
[CrossRef]

B. Bernhardt, A. Ozawa, P. Jacquet, M. Jacquey, Y. Kobayashi, T. Udem, R. Holzwarth, G. Guelachvili, T. W. Hänsch, and N. Picqué, Nat. Photonics 4, 55 (2010).
[CrossRef]

Jacquey, M.

B. Bernhardt, A. Ozawa, P. Jacquet, M. Jacquey, Y. Kobayashi, T. Udem, R. Holzwarth, G. Guelachvili, T. W. Hänsch, and N. Picqué, Nat. Photonics 4, 55 (2010).
[CrossRef]

Jones, D. J.

D. J. Jones, E. O. Potma, J. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, Rev. Sci. Instrum. 73, 2843 (2002).
[CrossRef]

Kippenberg, T. J.

C. Wang, T. Herr, P. Del’Haye, A. Schliesser, R. Holzwarth, T. W. Hänsch, N. Picqué, and T. J. Kippenberg, “Mid-infrared frequency combs based on crystalline microresonators,” arXiv:1109.2716 (2011).

Klein, T.

Kobayashi, Y.

B. Bernhardt, A. Ozawa, P. Jacquet, M. Jacquey, Y. Kobayashi, T. Udem, R. Holzwarth, G. Guelachvili, T. W. Hänsch, and N. Picqué, Nat. Photonics 4, 55 (2010).
[CrossRef]

Marx, B.

Mathies, R. A.

S. Shim and R. A. Mathies, J. Raman Spectrosc. 39, 1526 (2008).
[CrossRef]

Min, W.

C. W. Freudiger, M. B. J. Roeffaers, X. Zhang, B. G. Saar, W. Min, and X. S. Xie, J. Phys. Chem. B 115, 5574 (2011).
[CrossRef]

C. W. Freudiger, W. Min, G. R. Holtom, B. Xu, M. Dantus, and X. S. Xie, Nat. Photonics 5, 103 (2011).
[CrossRef]

Newbury, N. R.

E. Baumann, F. R. Giorgetta, W. C. Swann, A. M. Zolot, I. Coddington, and N. R. Newbury, Phys. Rev. A 84, 062513 (2011).
[CrossRef]

I. Coddington, W. C. Swann, and N. R. Newbury, Phys. Rev. Lett. 100, 013902 (2008).
[CrossRef]

Ozawa, A.

B. Bernhardt, A. Ozawa, P. Jacquet, M. Jacquey, Y. Kobayashi, T. Udem, R. Holzwarth, G. Guelachvili, T. W. Hänsch, and N. Picqué, Nat. Photonics 4, 55 (2010).
[CrossRef]

Pang, Y.

D. J. Jones, E. O. Potma, J. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, Rev. Sci. Instrum. 73, 2843 (2002).
[CrossRef]

Picqué, N.

A. Schliesser, N. Picqué, and T. W. Hänsch, Nat. Photonics 6, 440 (2012).
[CrossRef]

B. Bernhardt, E. Sorokin, P. Jacquet, R. Thon, T. Becker, I. T. Sorokina, N. Picqué, and T. W. Hänsch, Appl. Phys. B 100, 3 (2010).
[CrossRef]

B. Bernhardt, A. Ozawa, P. Jacquet, M. Jacquey, Y. Kobayashi, T. Udem, R. Holzwarth, G. Guelachvili, T. W. Hänsch, and N. Picqué, Nat. Photonics 4, 55 (2010).
[CrossRef]

T. Ideguchi, A. Poisson, G. Guelachvili, N. Picqué, and T. W. Hänsch, “Adaptive real-time dual-comb spectroscopy,” arXiv:1201.4177 (2012).

C. Wang, T. Herr, P. Del’Haye, A. Schliesser, R. Holzwarth, T. W. Hänsch, N. Picqué, and T. J. Kippenberg, “Mid-infrared frequency combs based on crystalline microresonators,” arXiv:1109.2716 (2011).

Ploetz, E.

Poisson, A.

T. Ideguchi, A. Poisson, G. Guelachvili, N. Picqué, and T. W. Hänsch, “Adaptive real-time dual-comb spectroscopy,” arXiv:1201.4177 (2012).

Potma, E. O.

D. J. Jones, E. O. Potma, J. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, Rev. Sci. Instrum. 73, 2843 (2002).
[CrossRef]

Roeffaers, M. B. J.

C. W. Freudiger, M. B. J. Roeffaers, X. Zhang, B. G. Saar, W. Min, and X. S. Xie, J. Phys. Chem. B 115, 5574 (2011).
[CrossRef]

Saar, B. G.

C. W. Freudiger, M. B. J. Roeffaers, X. Zhang, B. G. Saar, W. Min, and X. S. Xie, J. Phys. Chem. B 115, 5574 (2011).
[CrossRef]

Schliesser, A.

A. Schliesser, N. Picqué, and T. W. Hänsch, Nat. Photonics 6, 440 (2012).
[CrossRef]

C. Wang, T. Herr, P. Del’Haye, A. Schliesser, R. Holzwarth, T. W. Hänsch, N. Picqué, and T. J. Kippenberg, “Mid-infrared frequency combs based on crystalline microresonators,” arXiv:1109.2716 (2011).

Shim, S.

S. Shim and R. A. Mathies, J. Raman Spectrosc. 39, 1526 (2008).
[CrossRef]

Sorokin, E.

B. Bernhardt, E. Sorokin, P. Jacquet, R. Thon, T. Becker, I. T. Sorokina, N. Picqué, and T. W. Hänsch, Appl. Phys. B 100, 3 (2010).
[CrossRef]

Sorokina, I. T.

B. Bernhardt, E. Sorokin, P. Jacquet, R. Thon, T. Becker, I. T. Sorokina, N. Picqué, and T. W. Hänsch, Appl. Phys. B 100, 3 (2010).
[CrossRef]

Swann, W. C.

E. Baumann, F. R. Giorgetta, W. C. Swann, A. M. Zolot, I. Coddington, and N. R. Newbury, Phys. Rev. A 84, 062513 (2011).
[CrossRef]

I. Coddington, W. C. Swann, and N. R. Newbury, Phys. Rev. Lett. 100, 013902 (2008).
[CrossRef]

Thon, R.

B. Bernhardt, E. Sorokin, P. Jacquet, R. Thon, T. Becker, I. T. Sorokina, N. Picqué, and T. W. Hänsch, Appl. Phys. B 100, 3 (2010).
[CrossRef]

Udem, T.

B. Bernhardt, A. Ozawa, P. Jacquet, M. Jacquey, Y. Kobayashi, T. Udem, R. Holzwarth, G. Guelachvili, T. W. Hänsch, and N. Picqué, Nat. Photonics 4, 55 (2010).
[CrossRef]

Wang, C.

C. Wang, T. Herr, P. Del’Haye, A. Schliesser, R. Holzwarth, T. W. Hänsch, N. Picqué, and T. J. Kippenberg, “Mid-infrared frequency combs based on crystalline microresonators,” arXiv:1109.2716 (2011).

Xie, X. S.

C. W. Freudiger, M. B. J. Roeffaers, X. Zhang, B. G. Saar, W. Min, and X. S. Xie, J. Phys. Chem. B 115, 5574 (2011).
[CrossRef]

C. W. Freudiger, W. Min, G. R. Holtom, B. Xu, M. Dantus, and X. S. Xie, Nat. Photonics 5, 103 (2011).
[CrossRef]

D. J. Jones, E. O. Potma, J. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, Rev. Sci. Instrum. 73, 2843 (2002).
[CrossRef]

Xu, B.

C. W. Freudiger, W. Min, G. R. Holtom, B. Xu, M. Dantus, and X. S. Xie, Nat. Photonics 5, 103 (2011).
[CrossRef]

Ye, J.

D. J. Jones, E. O. Potma, J. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, Rev. Sci. Instrum. 73, 2843 (2002).
[CrossRef]

Zhang, X.

C. W. Freudiger, M. B. J. Roeffaers, X. Zhang, B. G. Saar, W. Min, and X. S. Xie, J. Phys. Chem. B 115, 5574 (2011).
[CrossRef]

Zolot, A. M.

E. Baumann, F. R. Giorgetta, W. C. Swann, A. M. Zolot, I. Coddington, and N. R. Newbury, Phys. Rev. A 84, 062513 (2011).
[CrossRef]

Appl. Phys. B (1)

B. Bernhardt, E. Sorokin, P. Jacquet, R. Thon, T. Becker, I. T. Sorokina, N. Picqué, and T. W. Hänsch, Appl. Phys. B 100, 3 (2010).
[CrossRef]

J. Phys. Chem. B (1)

C. W. Freudiger, M. B. J. Roeffaers, X. Zhang, B. G. Saar, W. Min, and X. S. Xie, J. Phys. Chem. B 115, 5574 (2011).
[CrossRef]

J. Raman Spectrosc. (1)

S. Shim and R. A. Mathies, J. Raman Spectrosc. 39, 1526 (2008).
[CrossRef]

Nat. Photonics (3)

B. Bernhardt, A. Ozawa, P. Jacquet, M. Jacquey, Y. Kobayashi, T. Udem, R. Holzwarth, G. Guelachvili, T. W. Hänsch, and N. Picqué, Nat. Photonics 4, 55 (2010).
[CrossRef]

C. W. Freudiger, W. Min, G. R. Holtom, B. Xu, M. Dantus, and X. S. Xie, Nat. Photonics 5, 103 (2011).
[CrossRef]

A. Schliesser, N. Picqué, and T. W. Hänsch, Nat. Photonics 6, 440 (2012).
[CrossRef]

Opt. Express (1)

Phys. Rev. A (1)

E. Baumann, F. R. Giorgetta, W. C. Swann, A. M. Zolot, I. Coddington, and N. R. Newbury, Phys. Rev. A 84, 062513 (2011).
[CrossRef]

Phys. Rev. Lett. (1)

I. Coddington, W. C. Swann, and N. R. Newbury, Phys. Rev. Lett. 100, 013902 (2008).
[CrossRef]

Rev. Mod. Phys. (1)

T. W. Hänsch, Rev. Mod. Phys. 78, 1297 (2006).
[CrossRef]

Rev. Sci. Instrum. (1)

D. J. Jones, E. O. Potma, J. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, Rev. Sci. Instrum. 73, 2843 (2002).
[CrossRef]

Other (2)

T. Ideguchi, A. Poisson, G. Guelachvili, N. Picqué, and T. W. Hänsch, “Adaptive real-time dual-comb spectroscopy,” arXiv:1201.4177 (2012).

C. Wang, T. Herr, P. Del’Haye, A. Schliesser, R. Holzwarth, T. W. Hänsch, N. Picqué, and T. J. Kippenberg, “Mid-infrared frequency combs based on crystalline microresonators,” arXiv:1109.2716 (2011).

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Figures (4)

Fig. 1.
Fig. 1.

Principle of RIKE dual-comb spectroscopy.

Fig. 2.
Fig. 2.

Experimental setup for RIKE dual-comb spectroscopy. x-Pol, crossed-polarizer; λ/4, quarter-wave plate; λ/2, half-wave plate; PZT, piezo-electric transducer; DAQ, data acquisition.

Fig. 3.
Fig. 3.

Experimental Raman gain amplitude and dispersion spectra of benzonitrile, measured within 293 μs. The phase of the pump laser is slowly varying and does not contribute to the resonance in the dispersion spectrum.

Fig. 4.
Fig. 4.

Experimental spectrum of p-Xylene.

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