We determine the absolute frequencies of 56 rotation-vibration transitions of the ν₃ band of CH₄ from 88.2 to 90.5 THz with a typical uncertainty of 2 kHz corresponding to a relative uncertainty of 2.2 × 10⁻¹¹ over an average time of a few hundred seconds. Saturated absorption lines are observed using a difference-frequency-generation source and a cavity-enhanced absorption cell, and the transition frequencies are measured with a fiber-laser-based optical frequency comb referenced to a rubidium atomic clock linked to the international atomic time. The determined value of the P(7) F₂⁽²⁾ line is consistent with the International Committee for Weights and Measures recommendation within the uncertainty.

© 2011 OSA

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16. A. G. Maki and J. S. Wells, “New wavenumber calibration tables from heterodyne frequency measurements,” J. Res. Natl. Inst. Stand. Technol. 97, 409–470 (1992).
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22. O. Tadanaga, T. Yanagawa, Y. Nishida, H. Miyazawa, K. Magari, M. Asobe, and H. Suzuki, “Efficient 3-μm difference frequency generation using direct-bonded quasi-phase-matched LiNbO3 ridge waveguides,” Appl. Phys. Lett. 88(6), 061101 (2006). [CrossRef]
23. D. J. Jones, S. A. Diddams, J. K. Ranka, A. Stentz, R. S. Windeler, J. L. Hall, and S. T. Cundiff, “Carrier-envelope phase control of femtosecond mode-locked lasers and direct optical frequency synthesis,” Science 288(5466), 635–639 (2000). [CrossRef] [PubMed]
24. T. Yasui, Y. Kabetani, E. Saneyoshi, S. Yokoyama, and T. Araki, “Terahertz frequency comb by multifrequency-heterodyning photoconductive detection for high-accuracy, high-resolution terahertz spectroscopy,” Appl. Phys. Lett. 88(24), 241104 (2006). [CrossRef]
25. T. J. Pinkert, D. Z. Kandula, C. Gohle, I. Barmes, J. Morgenweg, and K. S. E. Eikema, “Widely tunable extreme UV frequency comb generation,” Opt. Lett. 36(11), 2026–2028 (2011). [CrossRef] [PubMed]
26. D. Mazzotti, P. Cancio, A. Castrillo, I. Galli, G. Giusfredi, and P. De Natale, “A comb-referenced difference-frequency spectrometer for cavity ring-down spectroscopy in the 4.5 μm region,” J. Opt. A, Pure Appl. Opt. 8(7), S490–S493 (2006). [CrossRef]
27. P. Malara, P. Maddaloni, G. Gagliardi, and P. De Natale, “Absolute measurement of molecular transitions by a direct link to a comb generated around 3 μm,” Opt. Express 16(11), 8242–8249 (2008). [CrossRef] [PubMed]
28. P. Maddaloni, P. Malara, E. De Tommasi, M. De Rosa, I. Ricciardi, G. Gagliardi, F. Tamassia, G. Di Lonardo, and P. De Natale, “Absolute measurement of the S(0) and S(1) lines in the electric quadrupole fundamental band of D2 around 3μm,” J. Chem. Phys. 133(15), 154317 (2010). [CrossRef] [PubMed]
29. D. Mazzotti, P. Cancio, G. Giusfredi, P. De Natale, and M. Prevedelli, “Frequency-comb-based absolute frequency measurements in the mid-infrared with a difference-frequency spectrometer,” Opt. Lett. 30(9), 997–999 (2005). [CrossRef] [PubMed]
30. K. Takahata, T. Kobayashi, H. Sasada, Y. Nakajima, H. Inaba, and F. L. Hong, “The absolute frequency measurement of sub-Doppler molecular lines using a 3.4-μm difference-frequency-generation spectrometer and a fiber-based frequency comb,” Phys. Rev. A 80(3), 032518 (2009). [CrossRef]
31. G. Giusfredi, S. Bartalini, S. Borri, P. Cancio, I. Galli, D. Mazzotti, and P. De Natale, “Saturated-absorption cavity ring-down spectroscopy,” Phys. Rev. Lett. 104(11), 110801 (2010). [CrossRef] [PubMed]
32. M. Abe, K. Takahata, and H. Sasada, “Sub-Doppler resolution 3.4 microm spectrometer with an efficient difference-frequency-generation source,” Opt. Lett. 34(11), 1744–1746 (2009). [CrossRef] [PubMed]
33. T. R. Schibli, K. Minoshima, F. L. Hong, H. Inaba, A. Onae, H. Matsumoto, I. Hartl, and M. E. Fermann, “Frequency metrology with a turnkey all-fiber system,” Opt. Lett. 29(21), 2467–2469 (2004). [CrossRef] [PubMed]
34. H. Inaba, Y. Daimon, F. L. Hong, A. Onae, K. Minoshima, T. R. Schibli, H. Matsumoto, M. Hirano, T. Okuno, M. Onishi, and M. Nakazawa, “Long-term measurement of optical frequencies using a simple, robust and low-noise fiber based frequency comb,” Opt. Express 14(12), 5223–5231 (2006). [CrossRef] [PubMed]
35. J. Ye and J. L. Hall, “Absorption detection at the quantum limit: Probing high-finesse cavities with modulation techniques,” in Cavity-enhanced spectroscopy, Experimental methods in the physical sciences vol. 40, R. D. van Zee and J. P. Looney ed. (Academic Press, San Diego, 2002).
36. S. Okubo, H. Nakayama, and H. Sasada, “Hyperfine-resolved 3.4-μm spectroscopy of CH3I with a widely tunable frequency generation source and a cavity-enhanced cell: A case study of a local Coriolis interaction between the v1 = 1 and (v2, v6l) = (1, 22) states,” Phys. Rev. A 83(1), 012505 (2011). [CrossRef]
37. Y. Nakajima, H. Inaba, F. L. Hong, A. Onae, K. Minoshima, T. Kobayashi, M. Nakazawa, and H. Matsumoto, “Optimized amplification of femtosecond optical pulses by dispersion management for octave-spanning optical frequency comb generation,” Opt. Commun. 281(17), 4484–4487 (2008). [CrossRef]
38. R. L. Barger and J. L. Hall, “Pressure shift and broadening of methane line at 3.39 μ studied by laser-saturated molecular absorption,” Phys. Rev. Lett. 22(1), 4–8 (1969). [CrossRef]
39. E. V. Baklanov, B. Ya. Dubetskii, V. M. Semibalamut, and E. A. Titov, “Transit width of a nonlinear power resonance in low-pressure gases,” Sov. J. Quantum Electron. 5(11), 1374–1375 (1975). [CrossRef]
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41. L. Féjard, J. P. Champion, J. M. Jouvard, L. R. Brown, and A. S. Pine, “The Intensities of Methane in the 3-5 μm Region Revisited,” J. Mol. Spectrosc. 201, 83–94 (2000).
42. P. S. Ering, D. A. Tyurikov, G. Kramer, and B. Lipphardt, “Measurement of the absolute frequency of the methane E-line at 88 THz,” Opt. Commun. 151(4-6), 229–234 (1998). [CrossRef]
43. J. L. Hall and C. J. Bordé, “Shift and broadening of saturated absorption resonances due to curvature of the laser wave front,” Appl. Phys. Lett. 29(12), 788 (1976). [CrossRef]
44. M. Takami, K. Uehara, and K. Shimoda, “Rotational transitions of CH4 in the v3 = 1 excited state observed by an infrared-microwave double resonance method,” Jpn. J. Appl. Phys. 12(6), 924–925 (1973). [CrossRef]
45. R. F. Curl., “Infrared-radio frequency double resonance observations of pure rotational Q-branch transitions of methane,” J. Mol. Spectrosc. 48(1), 165–173 (1973). [CrossRef]
46. R. F. Curl, T. Oka, and D. S. Smith, “The observation of a pure rotational Q-branch transition of methane by infrared-radio frequency double resonance,” J. Mol. Spectrosc. 46(3), 518–520 (1973). [CrossRef]
47. C. J. Pursell and D. P. Weliky, “Pure rotational transitions in the v3 state of methane,” J. Mol. Spectrosc. 153(1-2), 303–306 (1992). [CrossRef]

Annu. Rev. Phys. Chem.

• M. Quack, J. Stohner, and M. Willeke, “High-resolution spectroscopic studies and theory of parity violation in chiral molecules,” Annu. Rev. Phys. Chem. 59(1), 741–769 (2008). [CrossRef] [PubMed]

Appl. Phys. B

• B. Meyer, S. Saupe, M. H. Wappelhorst, T. George, F. Kühnemann, M. Schneider, M. Havenith, W. Urban, and J. Legrand, “CO laser side-band spectrometer: Sub-Doppler heterodyne frequency measurements around 5 μm,” Appl. Phys. B 61, 169–173 (1995). [CrossRef]

Appl. Phys. Lett.

• G. Magerl, J. M. Frey, W. A. Kreiner, and T. Oka, “Inverse Lamb dip spectroscopy using microwave modulation sidebands of CO2 laser lines,” Appl. Phys. Lett. 42(8), 656–658 (1983). [CrossRef]
• O. Tadanaga, T. Yanagawa, Y. Nishida, H. Miyazawa, K. Magari, M. Asobe, and H. Suzuki, “Efficient 3-μm difference frequency generation using direct-bonded quasi-phase-matched LiNbO3 ridge waveguides,” Appl. Phys. Lett. 88(6), 061101 (2006). [CrossRef]
• T. Yasui, Y. Kabetani, E. Saneyoshi, S. Yokoyama, and T. Araki, “Terahertz frequency comb by multifrequency-heterodyning photoconductive detection for high-accuracy, high-resolution terahertz spectroscopy,” Appl. Phys. Lett. 88(24), 241104 (2006). [CrossRef]
• J. L. Hall and C. J. Bordé, “Shift and broadening of saturated absorption resonances due to curvature of the laser wave front,” Appl. Phys. Lett. 29(12), 788 (1976). [CrossRef]

Chirality

• B. Darquié, C. Stoeffler, A. Shelkovnikov, C. Daussy, A. Amy-Klein, C. Chardonnet, S. Zrig, L. Guy, J. Crassous, P. Soulard, P. Asselin, T. R. Huet, P. Schwerdtfeger, R. Bast, and T. Saue, “Progress toward the first observation of parity violation in chiral molecules by high-resolution laser spectroscopy,” Chirality 22(10), 870–884 (2010). [CrossRef] [PubMed]

J. Chem. Phys.

• P. Maddaloni, P. Malara, E. De Tommasi, M. De Rosa, I. Ricciardi, G. Gagliardi, F. Tamassia, G. Di Lonardo, and P. De Natale, “Absolute measurement of the S(0) and S(1) lines in the electric quadrupole fundamental band of D2 around 3μm,” J. Chem. Phys. 133(15), 154317 (2010). [CrossRef] [PubMed]
• A. Pine, “Self-, N2, O2, H2, Ar, and He broadening in the ν3 band Q branch of CH4,” J. Chem. Phys. 97(2), 773–785 (1992). [CrossRef]

J. Mol. Spectrosc.

• L. Féjard, J. P. Champion, J. M. Jouvard, L. R. Brown, and A. S. Pine, “The Intensities of Methane in the 3-5 μm Region Revisited,” J. Mol. Spectrosc. 201, 83–94 (2000).
• R. F. Curl., “Infrared-radio frequency double resonance observations of pure rotational Q-branch transitions of methane,” J. Mol. Spectrosc. 48(1), 165–173 (1973). [CrossRef]
• R. F. Curl, T. Oka, and D. S. Smith, “The observation of a pure rotational Q-branch transition of methane by infrared-radio frequency double resonance,” J. Mol. Spectrosc. 46(3), 518–520 (1973). [CrossRef]
• C. J. Pursell and D. P. Weliky, “Pure rotational transitions in the v3 state of methane,” J. Mol. Spectrosc. 153(1-2), 303–306 (1992). [CrossRef]
• T. George, W. Urban, and A. Le Floch, “Improved mass-independent Dunham parameters for the ground state of CO and calibration frequencies for the fundamental band,” J. Mol. Spectrosc. 165(2), 500–505 (1994). [CrossRef]
• A. Amy-Klein, H. Vigué, and C. Chardonnet, “Absolute frequency measurement of 12CO2 laser lines with a femtosecond laser comb and new determination of the 12CO2 molecular constants and frequency grid,” J. Mol. Spectrosc. 228(1), 206–212 (2004). [CrossRef]

J. Opt. A, Pure Appl. Opt.

• D. Mazzotti, P. Cancio, A. Castrillo, I. Galli, G. Giusfredi, and P. De Natale, “A comb-referenced difference-frequency spectrometer for cavity ring-down spectroscopy in the 4.5 μm region,” J. Opt. A, Pure Appl. Opt. 8(7), S490–S493 (2006). [CrossRef]

J. Quant. Spectrosc. Radiat. Transf.

• L. S. Rothman, I. E. Gordon, A. Barbe, D. Chris Benner, P. E. Bernath, M. Birk, V. Boudon, L. R. Brown, A. Campargue, J. P. Champion, K. Chance, L. H. Coudert, V. Dana, V. M. Devi, S. Fally, J.-M. Flaud, R. R. Gamache, A. Goldman, D. Jacquemart, I. Kleiner, N. Lacome, W. J. Lafferty, J.-Y. Mandin, S. T. Massie, S. N. Mikhailenko, C. E. Miller, N. Moazzen-Ahmadi, O. V. Naumenko, A. V. Nikitin, J. Orphal, V. I. Perevalov, A. Perrin, A. Predoi-Cross, C. P. Rinsland, M. Rotger, M. Simeckova, M. A. H. Smith, K. Sung, S. A. Tashukun, J. Tennyson, R. A. Toth, A. C. Vandaele, and J. Vander Auwera, “The HITRAN 2008 molecular spectroscopic database,” J. Quant. Spectrosc. Radiat. Transf. 110(9-10), 533–572 (2009). [CrossRef]
• N. Jacquinet-Husson, N. A. Scott, A. Chédin, L. Crépeau, R. Armante, V. Capelle, J. Orphal, A. Coustenis, C. Boonne, N. Poulet-Crovisier, A. Barbe, M. Birk, L. R. Brown, C. Camy-Peyret, C. Claveau, K. Chance, N. Christidis, C. Clerbaux, P. F. Coheur, V. Dana, L. Daumont, M. R. De Backer-Barilly, G. Di Lonardo, J. M. Flaud, A. Goldman, A. Hamdouni, M. Hess, M. D. Hurley, D. Jacquemart, I. Kleiner, P. Köpke, J. Y. Mandin, S. Massie, S. Mikhailenko, V. Nemtchinov, A. Nikitin, D. Newnham, A. Perrin, V. I. Perevalov, S. Pinnock, L. Régalia-Jarlot, C. P. Rinsland, A. Rublev, F. Schreier, L. Schult, K. M. Smith, S. A. Tashkun, J. L. Teffo, R. A. Toth, V. G. Tyuterev, J. Vander Auwera, P. Varanasi, and G. Wagner, “The GEISA spectroscopic database: Current and future archive for Earth and planetary atmosphere studies,” J. Quant. Spectrosc. Radiat. Transf. 109(6), 1043–1059 (2008). [CrossRef]

J. Res. Natl. Inst. Stand. Technol.

• A. G. Maki and J. S. Wells, “New wavenumber calibration tables from heterodyne frequency measurements,” J. Res. Natl. Inst. Stand. Technol. 97, 409–470 (1992).

Jpn. J. Appl. Phys.

• M. Takami, K. Uehara, and K. Shimoda, “Rotational transitions of CH4 in the v3 = 1 excited state observed by an infrared-microwave double resonance method,” Jpn. J. Appl. Phys. 12(6), 924–925 (1973). [CrossRef]

Metrologia

• T. J. Quinn, “Practical realization of the definition of the metre, including recommended radiations of other optical frequency standards (2001),” Metrologia 40(2), 103–133 (2003). [CrossRef]

Opt. Commun.

• Y. Nakajima, H. Inaba, F. L. Hong, A. Onae, K. Minoshima, T. Kobayashi, M. Nakazawa, and H. Matsumoto, “Optimized amplification of femtosecond optical pulses by dispersion management for octave-spanning optical frequency comb generation,” Opt. Commun. 281(17), 4484–4487 (2008). [CrossRef]
• P. S. Ering, D. A. Tyurikov, G. Kramer, and B. Lipphardt, “Measurement of the absolute frequency of the methane E-line at 88 THz,” Opt. Commun. 151(4-6), 229–234 (1998). [CrossRef]

Opt. Express

• H. Inaba, Y. Daimon, F. L. Hong, A. Onae, K. Minoshima, T. R. Schibli, H. Matsumoto, M. Hirano, T. Okuno, M. Onishi, and M. Nakazawa, “Long-term measurement of optical frequencies using a simple, robust and low-noise fiber based frequency comb,” Opt. Express 14(12), 5223–5231 (2006). [CrossRef] [PubMed]
• P. Malara, P. Maddaloni, G. Gagliardi, and P. De Natale, “Absolute measurement of molecular transitions by a direct link to a comb generated around 3 μm,” Opt. Express 16(11), 8242–8249 (2008). [CrossRef] [PubMed]
• J. T. Remillard, D. Uy, W. H. Weber, F. Capasso, C. Gmachl, A. L. Hutchinson, D. Sivco, J. Baillargeon, and A. Y. Cho, “Sub-Doppler resolution limited Lamb-dip spectroscopy of NO with a quantum cascade distributed feedback laser,” Opt. Express 7(7), 243–248 (2000). [CrossRef] [PubMed]

Opt. Lett.

• E. V. Kovalchuk, D. Dekorsy, A. I. Lvovsky, C. Braxmaier, J. Mlynek, A. Peters, and S. Schiller, “High-resolution Doppler-free molecular spectroscopy with a continuous-wave optical parametric oscillator,” Opt. Lett. 26(18), 1430–1432 (2001). [CrossRef] [PubMed]
• M. Abe, K. Takahata, and H. Sasada, “Sub-Doppler resolution 3.4 microm spectrometer with an efficient difference-frequency-generation source,” Opt. Lett. 34(11), 1744–1746 (2009). [CrossRef] [PubMed]
• T. R. Schibli, K. Minoshima, F. L. Hong, H. Inaba, A. Onae, H. Matsumoto, I. Hartl, and M. E. Fermann, “Frequency metrology with a turnkey all-fiber system,” Opt. Lett. 29(21), 2467–2469 (2004). [CrossRef] [PubMed]
• D. Mazzotti, P. Cancio, G. Giusfredi, P. De Natale, and M. Prevedelli, “Frequency-comb-based absolute frequency measurements in the mid-infrared with a difference-frequency spectrometer,” Opt. Lett. 30(9), 997–999 (2005). [CrossRef] [PubMed]
• T. J. Pinkert, D. Z. Kandula, C. Gohle, I. Barmes, J. Morgenweg, and K. S. E. Eikema, “Widely tunable extreme UV frequency comb generation,” Opt. Lett. 36(11), 2026–2028 (2011). [CrossRef] [PubMed]

Phys. Rev. A

• K. Takahata, T. Kobayashi, H. Sasada, Y. Nakajima, H. Inaba, and F. L. Hong, “The absolute frequency measurement of sub-Doppler molecular lines using a 3.4-μm difference-frequency-generation spectrometer and a fiber-based frequency comb,” Phys. Rev. A 80(3), 032518 (2009). [CrossRef]
• S. Okubo, H. Nakayama, and H. Sasada, “Hyperfine-resolved 3.4-μm spectroscopy of CH3I with a widely tunable frequency generation source and a cavity-enhanced cell: A case study of a local Coriolis interaction between the v1 = 1 and (v2, v6l) = (1, 22) states,” Phys. Rev. A 83(1), 012505 (2011). [CrossRef]

Phys. Rev. Lett.

• G. Giusfredi, S. Bartalini, S. Borri, P. Cancio, I. Galli, D. Mazzotti, and P. De Natale, “Saturated-absorption cavity ring-down spectroscopy,” Phys. Rev. Lett. 104(11), 110801 (2010). [CrossRef] [PubMed]
• R. L. Barger and J. L. Hall, “Pressure shift and broadening of methane line at 3.39 μ studied by laser-saturated molecular absorption,” Phys. Rev. Lett. 22(1), 4–8 (1969). [CrossRef]
• J. L. Hall, C. J. Bordé, and K. Uehara, “Direct optical resolution of the recoil effect using saturated absorption spectroscopy,” Phys. Rev. Lett. 37(20), 1339–1342 (1976). [CrossRef]
• C. Daussy, T. Marrel, A. Amy-Klein, C. T. Nguyen, C. J. Bordé, and C. Chardonnet, “Limit on the parity nonconserving energy difference between the enantiomers of a chiral molecule by laser spectroscopy,” Phys. Rev. Lett. 83(8), 1554–1557 (1999). [CrossRef]
• C. Daussy, M. Guinet, A. Amy-Klein, K. Djerroud, Y. Hermier, S. Briaudeau, ChJ. Bordé, and C. Chardonnet, “Direct determination of the Boltzmann constant by an optical method,” Phys. Rev. Lett. 98(25), 250801 (2007). [CrossRef] [PubMed]
• G. Casa, A. Castrillo, G. Galzerano, R. Wehr, A. Merlone, D. Di Serafino, P. Laporta, and L. Gianfrani, “Primary gas thermometry by means of laser-absorption spectroscopy: determination of the Boltzmann constant,” Phys. Rev. Lett. 100(20), 200801 (2008). [CrossRef] [PubMed]

Science

• D. J. Jones, S. A. Diddams, J. K. Ranka, A. Stentz, R. S. Windeler, J. L. Hall, and S. T. Cundiff, “Carrier-envelope phase control of femtosecond mode-locked lasers and direct optical frequency synthesis,” Science 288(5466), 635–639 (2000). [CrossRef] [PubMed]

Sov. J. Quantum Electron.

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