Abstract

Cavity-enhanced spectroscopic instruments impact a broad range of scientific fields because they are sensitive, self-contained, and can be packaged for use by nonspecialists. Infrared-laser-based cavity-enhanced instruments are typically limited to measuring a few small molecules because they rely on narrowly tunable lasers that each measure a molecular transition. Broadband dual-comb spectroscopy (DCS) is a spectroscopic technique capable of simultaneously probing molecular absorption on thousands of narrowly spaced wavelengths using a single high-speed photodetector. With coherent averaging, DCS can measure multiple species, including large molecules, with a high signal-to-noise ratio (SNR). Here, we lock a high-finesse optical cavity to a broadband mode-locked frequency comb with an approach that enables a high SNR, broadband cavity-enhanced DCS with coherent averaging. With a 7.5 cm optical cavity, we attain a >12,000× path-length-enhancement factor, 60 nm bandwidth near 1660 nm (3.5% fractional bandwidth), and >27  dB SNR in 160 s. We measure the dense rovibrational spectrum of ethane in a background of overlapping H2O, CH4, and CO2 absorption. By combining the broadband, high-resolution, and single-detector nature of DCS with a compact optical cavity, we enable future self-contained instruments that are able to simultaneously detect a variety of molecules in realistic ambient conditions.

© 2019 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

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2018 (6)

Z. Chen, M. Yan, T. W. Hänsch, and N. Picqué, “A phase-stable dual-comb interferometer,” Nat. Commun. 9, 3035 (2018).
[Crossref]

S. Coburn, C. B. Alden, R. Wright, K. Cossel, E. Baumann, G.-W. Truong, F. Giorgetta, C. Sweeney, N. R. Newbury, K. Prasad, I. Coddington, and G. B. Rieker, “Continuous regional trace-gas source attribution using a field-deployed dual frequency comb spectrometer,” Optica 5, 320–327 (2018).
[Crossref]

A. J. Fleisher, D. A. Long, and J. T. Hodges, “Quantitative modeling of complex molecular response in coherent cavity-enhanced dual-comb spectroscopy,” J. Mol. Spectrosc. 352, 26–35 (2018).
[Crossref]

H. Timmers, A. Kowligy, A. Lind, F. C. Cruz, N. Nader, M. Silfies, G. Ycas, T. K. Allison, P. G. Schunemann, S. B. Papp, and S. A. Diddams, “Molecular fingerprinting with bright, broadband infrared frequency combs,” Optica 5, 727–732 (2018).
[Crossref]

G. Ycas, F. R. Giorgetta, E. Baumann, I. Coddington, D. Herman, S. A. Diddams, and N. R. Newbury, “High coherence mid-infrared dual comb spectroscopy spanning 2.6 to 5.2 microns,” Nat. Photonics 12, 202–208 (2018).
[Crossref]

A. V. Muraviev, V. O. Smolski, Z. E. Loparo, and K. L. Vodopyanov, “Massively parallel sensing of trace molecules and their isotopologues with broadband subharmonic mid-infrared frequency combs,” Nat. Photonics 12, 209–214 (2018).
[Crossref]

2017 (4)

L. Rutkowski, A. C. Johansson, G. Zhao, T. Hausmaninger, A. Khodabakhsh, O. Axner, and A. Foltynowicz, “Sensitive and broadband measurement of dispersion in a cavity using a Fourier transform spectrometer with kHz resolution,” Opt. Express 25, 21711–21718 (2017).
[Crossref]

S. M. Link, D. J. H. C. Maas, D. Waldburger, and U. Keller, “Dual-comb spectroscopy of water vapor with a free-running semiconductor disk laser,” Science 356, 1164–1168 (2017).
[Crossref]

A. Ozawa, J. Davila-Rodriguez, J. R. Bounds, H. A. Schuessler, T. W. Hänsch, and T. Udem, “Single ion fluorescence excited with a single mode of an UV frequency comb,” Nat. Commun. 8, 44 (2017).
[Crossref]

A. Khodabakhsh, L. Rutkowski, J. Morville, and A. Foltynowicz, “Mid-infrared continuous-filtering Vernier spectroscopy using a doubly resonant optical parametric oscillator,” Appl. Phys. B 123, 210 (2017).
[Crossref]

2016 (4)

A. M. Jayich, X. Long, and W. C. Campbell, “Direct frequency comb laser cooling and trapping,” Phys. Rev. X 6, 041004 (2016).
[Crossref]

A. J. Fleisher, D. A. Long, Z. D. Reed, J. T. Hodges, and D. F. Plusquellic, “Coherent cavity-enhanced dual-comb spectroscopy,” Opt. Express 24, 10424–10434 (2016).
[Crossref]

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

T. Ideguchi, T. Nakamura, Y. Kobayashi, and K. Goda, “Kerr-lens mode-locked bidirectional dual-comb ring laser for broadband dual-comb spectroscopy,” Optica 3, 748–753 (2016).
[Crossref]

2015 (3)

Z. D. Reed and J. T. Hodges, “Self- and air-broadened cross sections of ethane (C2H6) determined by frequency-stabilized cavity ring-down spectroscopy near 1.68 μm,” J. Quant. Spectrosc. Radiat. Transfer 159, 87–93 (2015).
[Crossref]

G. Millot, S. Pitois, M. Yan, T. Hovhannisyan, A. Bendahmane, T. W. Hänsch, and N. Picqué, “Frequency-agile dual-comb spectroscopy,” Nat. Photonics 10, 27–30 (2015).
[Crossref]

E. Portuondo-Campa, G. Buchs, S. Kundermann, L. Balet, and S. Lecomte, “Ultra-low phase-noise microwave generation using a diode-pumped solid-state laser based frequency comb and a polarization-maintaining pulse interleaver,” Opt. Express 23, 32441–32451 (2015).
[Crossref]

2014 (3)

2013 (5)

L. S. Rothman, I. E. Gordon, Y. Babikov, A. Barbe, D. Chris Benner, P. F. Bernath, M. Birk, L. Bizzocchi, V. Boudon, L. R. Brown, A. Campargue, K. Chance, E. A. Cohen, L. H. Coudert, V. M. Devi, B. J. Drouin, A. Fayt, J. M. Flaud, R. R. Gamache, J. J. Harrison, J. M. Hartmann, C. Hill, J. T. Hodges, D. Jacquemart, A. Jolly, J. Lamouroux, R. J. Le Roy, G. Li, D. A. Long, O. M. Lyulin, C. J. Mackie, S. T. Massie, S. Mikhailenko, H. S. P. Müller, O. V. Naumenko, A. V. Nikitin, J. Orphal, V. Perevalov, A. Perrin, E. R. Polovtseva, C. Richard, M. A. H. Smith, E. Starikova, K. Sung, S. Tashkun, J. Tennyson, G. C. Toon, V. G. Tyuterev, and G. Wagner, “The HITRAN2012 molecular spectroscopic database,” J. Quant. Spectrosc. Radiat. Transfer 130, 4–50 (2013).
[Crossref]

A. Foltynowicz, P. Masłowski, A. J. Fleisher, B. J. Bjork, and J. Ye, “Cavity-enhanced optical frequency comb spectroscopy in the mid-infrared application to trace detection of hydrogen peroxide,” Appl. Phys. B 110, 163–175 (2013).
[Crossref]

A. M. Zolot, F. R. Giorgetta, E. Baumann, W. C. Swann, I. Coddington, and N. R. Newbury, “Broad-band frequency references in the near-infrared: accurate dual comb spectroscopy of methane and acetylene,” J. Quant. Spectrosc. Radiat. Transfer 118, 26–39 (2013).
[Crossref]

S. Potvin and J. Genest, “Dual-comb spectroscopy using frequency-doubled combs around 775 nm,” Opt. Express 21, 30707–30715 (2013).
[Crossref]

A. J. Metcalf, V. Torres-Company, D. E. Leaird, and A. M. Weiner, “High-power broadly tunable electrooptic frequency comb generator,” IEEE J. Sel. Top. Quantum Electron. 19, 231–236 (2013).
[Crossref]

2012 (3)

A. Hugi, G. Villares, S. Blaser, H. C. Liu, and J. Faist, “Mid-infrared frequency comb based on a quantum cascade laser,” Nature 492, 229–233 (2012).
[Crossref]

J. Roy, J.-D. Deschênes, S. Potvin, and J. Genest, “Continuous real-time correction and averaging for frequency comb interferometry,” Opt. Express 20, 21932–21939 (2012).
[Crossref]

R. Grilli, G. Méjean, S. Kassi, I. Ventrillard, C. Abd-Alrahman, and D. Romanini, “Frequency comb based spectrometer for in situ and real time measurements of IO, BrO, NO2, and H2CO at pptv and ppqv levels,” Environ. Sci. Technol. 46, 10704–10710 (2012).
[Crossref]

2011 (3)

T. J. Kippenberg, R. Holzwarth, and S. A. Diddams, “Microresonator-based optical frequency combs,” Science 332, 555–559 (2011).
[Crossref]

T. M. Fortier, M. S. Kirchner, F. Quinlan, J. Taylor, J. C. Bergquist, T. Rosenband, N. Lemke, A. Ludlow, Y. Jiang, C. W. Oates, and S. A. Diddams, “Generation of ultrastable microwaves via optical frequency division,” Nat. Photonics 5, 425–429 (2011).
[Crossref]

A. Foltynowicz, T. Ban, P. Masłowski, F. Adler, and J. Ye, “Quantum-noise-limited optical frequency comb spectroscopy,” Phys. Rev. Lett. 107, 233002 (2011).
[Crossref]

2010 (3)

I. Coddington, W. C. Swann, and N. R. Newbury, “Coherent dual-comb spectroscopy at high signal-to-noise ratio,” Phys. Rev. A 82, 043817 (2010).
[Crossref]

B. Bernhardt, A. Ozawa, P. Jacquet, M. Jacquey, Y. Kobayashi, T. Udem, R. Holzwarth, G. Guelachvili, T. W. Hänsch, and N. Picqué, “Cavity-enhanced dual-comb spectroscopy,” Nat. Photonics 4, 55–57 (2010).
[Crossref]

N. R. Newbury, I. Coddington, and W. Swann, “Sensitivity of coherent dual-comb spectroscopy,” Opt. Express 18, 7929–7945 (2010).
[Crossref]

2009 (2)

2008 (1)

C. H. Li, A. J. Benedick, P. Fendel, A. G. Glenday, F. X. Kärtner, D. F. Phillips, D. Sasselov, A. Szentgyorgyi, and R. L. Walsworth, “A laser frequency comb that enables radial velocity measurements with a precision of 1  cm s-1,” Nature 452, 610–612 (2008).
[Crossref]

2007 (2)

C. Gohle, B. Stein, A. Schliesser, T. Udem, and T. W. Hänsch, “Frequency comb Vernier spectroscopy for broadband, high-resolution, high-sensitivity absorption and dispersion spectra,” Phys. Rev. Lett. 99, 263902 (2007).
[Crossref]

P. Del’Haye, A. Schliesser, O. Arcizet, T. Wilken, R. Holzwarth, and T. J. Kippenberg, “Optical frequency comb generation from a monolithic microresonator,” Nature 450, 1214–1217 (2007).
[Crossref]

2006 (2)

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M. G. Suh, Q. F. Yang, K. Y. Yang, X. Yi, and K. J. Vahala, “Microresonator soliton dual-comb spectroscopy,” Science 354, 600–603 (2016).
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A. Ozawa, J. Davila-Rodriguez, J. R. Bounds, H. A. Schuessler, T. W. Hänsch, and T. Udem, “Single ion fluorescence excited with a single mode of an UV frequency comb,” Nat. Commun. 8, 44 (2017).
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A. V. Muraviev, V. O. Smolski, Z. E. Loparo, and K. L. Vodopyanov, “Massively parallel sensing of trace molecules and their isotopologues with broadband subharmonic mid-infrared frequency combs,” Nat. Photonics 12, 209–214 (2018).
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Nature (5)

P. Del’Haye, A. Schliesser, O. Arcizet, T. Wilken, R. Holzwarth, and T. J. Kippenberg, “Optical frequency comb generation from a monolithic microresonator,” Nature 450, 1214–1217 (2007).
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C. H. Li, A. J. Benedick, P. Fendel, A. G. Glenday, F. X. Kärtner, D. F. Phillips, D. Sasselov, A. Szentgyorgyi, and R. L. Walsworth, “A laser frequency comb that enables radial velocity measurements with a precision of 1  cm s-1,” Nature 452, 610–612 (2008).
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A. Foltynowicz, T. Ban, P. Masłowski, F. Adler, and J. Ye, “Quantum-noise-limited optical frequency comb spectroscopy,” Phys. Rev. Lett. 107, 233002 (2011).
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C. Gohle, B. Stein, A. Schliesser, T. Udem, and T. W. Hänsch, “Frequency comb Vernier spectroscopy for broadband, high-resolution, high-sensitivity absorption and dispersion spectra,” Phys. Rev. Lett. 99, 263902 (2007).
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Other (2)

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Supplementary Material (1)

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Figures (4)

Fig. 1.
Fig. 1. Schematic of the cavity–comb locking approach. Combs are fully stabilized by phase locking two comb teeth of each comb to two cavity-stabilized CW lasers. A tunable, high-SNR cavity lock is used to indirectly lock the cavity to the comb. The light from comb 1 ( f rep = f 1 ) is coupled to the high-finesse enhancement cavity where it interacts with the gas sample. The cavity-transmitted light beats with comb 2 ( f rep = f 1 + Δ f ) on a fast detector. The downconverted signal is then digitized with a 250 MS/s data acquisition card and processed. (a) Locking approach from spectral perspective. (b) Experimental schematic.
Fig. 2.
Fig. 2. Baseline-corrected absorbance of methane averaged for 11 s. Cavity mirror and molecular dispersion result in a variable frequency offset between the cavity and comb modes, which introduce a predictable distortion to the molecular line shape. The fitting routine accounts for the line shape distortion to infer methane concentration.
Fig. 3.
Fig. 3. (a) Baseline-corrected absorbance spectrum of a gas mixture (black) including C 2 H 6 , CH 4 , CO 2 , and H 2 O and the fit to the data (blue) using our multi-species fitting routine. (b) Fit residual. (c) Real part of the complex absorbance model of molecular species in the gas mixture. (d) Frequency offset between comb lines and cavity modes across the spectrum. The frequency offset is due to the cavity mirror dispersion. The zero crossing of the dispersion curve is around 1660 nm (180.5 THz), which matches well with the dispersion curves provided by the mirror manufacturer.
Fig. 4.
Fig. 4. Detection precision (modified Allan deviation) of C 2 H 6 . C 2 H 6 precision is 500 ppb after 160 s of averaging. C 2 H 6 precision (blue) follows 1 / τ 0.8 line (gray).