The sensitivity of molecular fingerprinting is dramatically improved when the absorbing sample is placed in a high-finesse optical cavity, because the effective path length is increased. When the equidistant lines from a laser frequency comb are simultaneously injected into the cavity over a large spectral range, multiple trace gases may be identified1 within a few milliseconds. However, efficient analysis of the light transmitted through the cavity remains challenging. Here, a novel approach—cavity-enhanced, frequency-comb, Fourier-transform spectroscopy—fully overcomes this difficulty and enables measurement of ultrasensitive, broad-bandwidth, high-resolution spectra within a few tens of microseconds without any need for detector arrays, potentially from the terahertz to ultraviolet regions. Within a period of just 18 µs, we recorded the spectra of the ammonia 1.0 µm overtone bands comprising 1,500 spectral elements and spanning 20 nm, with a resolution of 4.5 GHz and a noise equivalent absorption at 1 s averaging of 1 × 10−10 cm−1 Hz−1/2, thus opening a route to time-resolved spectroscopy of rapidly evolving single events.
Subscribe to Journal
Get full journal access for 1 year
only $4.92 per issue
All prices are NET prices.
VAT will be added later in the checkout.
Tax calculation will be finalised during checkout.
Rent or Buy article
Get time limited or full article access on ReadCube.
All prices are NET prices.
Thorpe, M. J., Moll, K. D., Jones, R. J., Safdi, B. & Ye, J. Broadband cavity ringdown spectroscopy for sensitive and rapid molecular detection. Science 311, 1595–1599 (2006).
Berden, G. & Engeln, R. eds. Cavity Ring Down Spectroscopy: Techniques and Applications (Wiley, September 2009).
Berden, G., Peeters, R. & Meijer, G. Cavity ring-down spectroscopy: experimental schemes and applications. Int. Rev. Phys. Chem. 19, 565–607 (2000).
Thorpe, M. J., Hudson, D. D., Moll, K. D., Lasri, J. & Ye, J. Cavity-ringdown molecular spectroscopy based on an optical frequency comb at 1.45–1.65 µm. Opt. Lett. 32, 307–309 (2007).
Thorpe, M. J. & Ye, J. Cavity-enhanced direct frequency comb spectroscopy. Appl. Phys. B 91, 397–414 (2008).
Thorpe, M. J., Balslev Clausen, D., Kirchner, M. S. & Ye, J. Cavity-enhanced optical frequency comb spectroscopy: application to human breath analysis. Opt. Express 16, 2387–2397 (2008).
Thorpe, M. J., Adler, F., Cossel, K. C., de Miranda, M. H. G. & Ye, J. Tomography of a supersonically cooled molecular jet using cavity-enhanced direct frequency comb spectroscopy. Chem. Phys. Lett. 468, 1–8 (2009).
Gohle, Ch., Stein, B., Schliesser, A., Udem, T. & Hänsch, T. W. Frequency comb Vernier spectroscopy for broadband, high-resolution, high-sensitivity absorption and dispersion spectra. Phys. Rev. Lett. 99, 263902 (2007).
Diddams, S. A., Hollberg, L. & Mbele, V. Molecular fingerprinting with the resolved modes of a femtosecond laser frequency comb. Nature 445, 627–630 (2007).
Bernhardt, B. et al. Laser frequency combs for molecular fingerprinting. 2009 IEEE LEOS Annual Meeting Conference Proceedings, IEEE Lasers and Electro-Optics Society (LEOS) Annual Meeting (2009).
Jacquet, P. et al. Frequency comb Fourier transform spectroscopy with kHz optical resolution, in Fourier Transform Spectroscopy paper FMB2, ThB4, 2 pp. (Optical Society of America, 2009).
Coddington, I., Swann, W. C. & Newbury, N. R. Coherent multiheterodyne spectroscopy using stabilized optical frequency combs. Phys. Rev. Lett. 100, 013902 (2008).
Ganz, T., Brehm, M., von Ribbeck, H. G., van der Weide, D. W. & Keilmann, F. Vector frequency-comb Fourier-transform spectroscopy for characterizing metamaterials. New J. Phys. 10, 123007 (2008).
Giaccari, P., Deschênes, J.-D., Saucier, P., Genest, J. & Tremblay, P. Active Fourier-transform spectroscopy combining the direct RF beating of two fiber-based mode-locked lasers with a novel referencing method. Opt. Express 16, 4347–4365 (2008).
Schliesser, A., Brehm, M., Keilmann, F. & van der Weide, D. W. Frequency-comb infrared spectrometer for rapid, remote chemical sensing. Opt. Express 13, 9029–9038 (2005).
Yasui, T., Saneyoshi, E. & Araki, T. Asynchronous optical sampling terahertz time-domain spectroscopy for ultrahigh spectral resolution and rapid data acquisition. Appl. Phys. Lett. 87, 061101 (2005).
Keilmann, F., Gohle, Ch. & Holzwarth, R. Time-domain mid-infrared frequency-comb spectrometer. Opt. Lett. 29, 1542–1544 (2004).
Schiller, S. Spectrometry with frequency combs. Opt. Lett. 27, 766–768 (2002).
Hänsch, T. W. Nobel lecture: passion for precision. Rev. Mod. Phys. 78, 1297–1309 (2006).
Udem, T., Holzwarth, R. & Hänsch, T. W. Optical frequency metrology. Nature 416, 233–237 (2002).
Drever, R. W. P. et al. Laser phase and frequency stabilization using an optical resonator. Appl. Phys. B 31, 97–105 (1983).
Herman, M., Huet, T. R. & Vervloet, M. Spectroscopy and vibrational couplings in the 3ν3 region of acetylene. Mol. Phys. 66, 333–353 (1989).
Irwin, P. G. J. et al. Band parameters and k coefficients for self-broadened ammonia in the range 4,000–11,000 cm−1. J. Quant. Spectrosc. Radiat. Transf. 62, 193–204 (1999).
Kleiner, I. et al. NH3 and PH3 line parameters: the 2000 HITRAN update and new results. J. Quant. Spectrosc. Radiat. Transf. 82, 293–312 (2003).
Adler, F. et al. Phase-stabilized 1.5 W frequency comb at 2.8–4.8 µm. Opt. Lett. 34, 1330–1332 (2009).
Research was conducted in the scope of the European Associated Laboratory ‘European Laboratory for Frequency Comb Spectroscopy’. Support was provided by the Max Planck Foundation and, for the PhD fellowship of P.J., by the Délégation Générale de l'Armement. The expert help of D. Höfling and T. Wilken in the operation of the ytterbium lasers is warmly acknowledged.
The authors declare no competing financial interests.
About this article
Cite this article
Bernhardt, B., Ozawa, A., Jacquet, P. et al. Cavity-enhanced dual-comb spectroscopy. Nature Photon 4, 55–57 (2010). https://doi.org/10.1038/nphoton.2009.217
Analytical Chemistry (2021)
OSA Continuum (2021)
Achieving Precise Spectral Analysis and Imaging Simultaneously with a Mode-Resolved Dual-Comb Interferometer
Rapid and precise partial pressure measurement of multiple gas species with mid-infrared electro-optic dual-comb spectroscopy
Femtosecond dual-comb Yb:CaF2 laser from a single free-running polarization-multiplexed cavity for optical sampling applications
Optics Express (2020)