This work presents a very simple yet effective way to obtain direct referencing of a quantum-cascade-laser at 4.3 μm to a near-IR frequency-comb. Precise tuning of the comb repetition-rate allows the quantum-cascade-laser to be scanned across absorption lines of a CO₂ gaseous sample and line profiles to be acquired with extreme reproducibility and accuracy. By averaging over 50 acquisitions, line-centre frequencies are retrieved with an uncertainty of 30 kHz in a linear interaction regime. The extension of this methodology to other lines and molecules, by the use of widely tunable extended-cavity quantum-cascade-lasers, paves the way to a wide availability of high-quality and traceable spectroscopic data in the most crucial region for molecular detection and interrogation.

© 2011 OSA

1. Th. Udem, R. Holzwarth, and T. W. Hänsch, “Optical frequency metrology,” Nature416(6877), 233–237 (2002). [CrossRef] [PubMed]
2. 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,” Science288(5466), 635–640 (2000). [CrossRef] [PubMed]
3. Th. Udem, R. Holzwarth, and T. W. Hansch, “Femtosecond optical frequency combs,” Eur. Phys. J. Spec. Top.172(1), 69–79 (2009). [CrossRef]
4. J. Faist, F. Capasso, D. L. Sivco, C. Sirtori, A. L. Hutchinson, and A. Y. Cho, “Quantum cascade laser,” Science264(5158), 553–556 (1994). [CrossRef] [PubMed]
5. M. Beck, D. Hofstetter, T. Aellen, J. Faist, U. Oesterle, M. Ilegems, E. Gini, and H. Melchior, “Continuous Wave Operation of a Mid-Infrared Semiconductor Laser at Room Temperature,” Science295(5553), 301–305 (2002). [CrossRef] [PubMed]
6. A. Hugi, R. Maulini, and J. Faist, “External cavity quantum cascade laser,” Semicond. Sci. Technol.25(8), 083001 (2010). [CrossRef]
7. A. Amy-Klein, A. Goncharov, C. Daussy, C. Grain, O. Lopez, G. Santarelli, and C. Chardonnet, “Absolute frequency measurement in the 28-THz spectral region with a femtosecond laser comb and a long-distance optical link to a primary standard,” Appl. Phys. B78(1), 25–30 (2004). [CrossRef]
8. P. Malara, P. Maddaloni, G. Gagliardi, and P. De Natale, “Absolute frequency measurement of molecular transitions by a direct link to a comb generated around 3-microm,” Opt. Express16(11), 8242–8249 (2008). [CrossRef] [PubMed]
9. 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]
10. S. Bartalini, S. Borri, P. Cancio, A. Castrillo, I. Galli, G. Giusfredi, D. Mazzotti, L. Gianfrani, and P. De Natale, “Observing the intrinsic linewidth of a quantum-cascade laser: beyond the Schawlow-Townes limit,” Phys. Rev. Lett.104(8), 083904 (2010). [CrossRef] [PubMed]
11. S. Bartalini, P. Cancio, G. Giusfredi, D. Mazzotti, P. De Natale, S. Borri, I. Galli, T. Leveque, and L. Gianfrani, “Frequency-comb-referenced quantum-cascade laser at 4.4 microm,” Opt. Lett.32(8), 988–990 (2007). [CrossRef] [PubMed]
12. M. Zimmermann, C. Gohle, R. Holzwarth, Th. Udem, and T. W. Hansch, “Optical clockwork with an offset-free difference-frequency comb: accuracy of sum- and difference-frequency generation,” Opt. Lett.29(3), 310–312 (2004). [CrossRef] [PubMed]
13. S. M. Foreman, A. Marian, J. Ye, E. A. Petrukhin, M. A. Gubin, O. D. Mücke, F. N. C. Wong, E. P. Ippen, and F. X. Kärtner, “Demonstration of a HeNe/CH4-based optical molecular clock,” Opt. Lett.30(5), 570–572 (2005). [CrossRef] [PubMed]
14. A. Amy-Klein, A. Goncharov, M. Guinet, C. Daussy, O. Lopez, A. Shelkovnikov, and C. Chardonnet, “Absolute frequency measurement of a SF6 two-photon line by use of a femtosecond optical comb and sum-frequency generation,” Opt. Lett.30(24), 3320–3322 (2005). [CrossRef] [PubMed]
15. J. Jiang, A. Onae, H. Matsumoto, and F. L. Hong, “Frequency measurement of acetylene-stabilized lasers using a femtosecond optical comb without carrier-envelope offset frequency control,” Opt. Express13(6), 1958–1965 (2005). [CrossRef] [PubMed]
16. C. Erny, K. Moutzouris, J. Biegert, D. Kühlke, F. Adler, A. Leitenstorfer, and U. Keller, “Mid-infrared difference-frequency generation of ultrashort pulses tunable between 3.2 and 4.8 microm from a compact fiber source,” Opt. Lett.32(9), 1138–1140 (2007). [CrossRef] [PubMed]
17. A. Gambetta, R. Ramponi, and M. Marangoni, “Mid-infrared optical combs from a compact amplified Er-doped fiber oscillator,” Opt. Lett.33(22), 2671–2673 (2008). [CrossRef] [PubMed]
18. T. A. Johnson and S. A. Diddams, “Mid-IR Frequency Comb Upconversion Spectroscopy”, in Conference on Lasers and Electro-Optics, OSA Technical Digest (CD) (Optical Society of America, 2010), paper CPDB11.
19. F. Adler, A. Sell, F. Sotier, R. Huber, and A. Leitenstorfer, “Attosecond relative timing jitter and 13 fs tunable pulses from a two-branch Er:fiber laser,” Opt. Lett.32(24), 3504–3506 (2007). [CrossRef] [PubMed]
20. F. Tauser, F. Adler, and A. Leitenstorfer, “Widely tunable sub-30-fs pulses from a compact erbium-doped fiber source,” Opt. Lett.29(5), 516–518 (2004). [CrossRef] [PubMed]
21. S. Barbieri, P. Gellie, G. Santarelli, L. Ding, W. Maineult, C. Sirtori, R. Colombelli, H. Beere, and D. Ritchie, “Phase-locking of a 2.7-THz quantum cascade laser to a mode-locked erbium-doped fibre laser,” Nat. Photonics4(9), 636–640 (2010). [CrossRef]
22. P. Gaal, M. B. Raschke, K. Reimann, and M. Woerner, “Measuring optical frequencies in the 0–40 THz range with non-synchronized electro–optic sampling,” Nat. Photonics1(10), 577–580 (2007). [CrossRef]
23. G. Casa, D. A. Parretta, A. Castrillo, R. Wehr, and L. Gianfrani, “Highly accurate determinations of CO2 line strengths using intensity-stabilized diode laser absorption spectrometry,” J. Chem. Phys.127(8), 084311 (2007). [CrossRef] [PubMed]
24. A. Castrillo, E. De Tommasi, L. Gianfrani, L. Sirigu, and J. Faist, “Doppler-free saturated-absorption spectroscopy of CO2 at 4.3 microm by means of a distributed feedback quantum cascade laser,” Opt. Lett.31(20), 3040–3042 (2006). [CrossRef] [PubMed]

Appl. Phys. B

• A. Amy-Klein, A. Goncharov, C. Daussy, C. Grain, O. Lopez, G. Santarelli, and C. Chardonnet, “Absolute frequency measurement in the 28-THz spectral region with a femtosecond laser comb and a long-distance optical link to a primary standard,” Appl. Phys. B78(1), 25–30 (2004). [CrossRef]

Eur. Phys. J. Spec. Top.

• Th. Udem, R. Holzwarth, and T. W. Hansch, “Femtosecond optical frequency combs,” Eur. Phys. J. Spec. Top.172(1), 69–79 (2009). [CrossRef]

J. Chem. Phys.

• G. Casa, D. A. Parretta, A. Castrillo, R. Wehr, and L. Gianfrani, “Highly accurate determinations of CO2 line strengths using intensity-stabilized diode laser absorption spectrometry,” J. Chem. Phys.127(8), 084311 (2007). [CrossRef] [PubMed]

Nat. Photonics

• S. Barbieri, P. Gellie, G. Santarelli, L. Ding, W. Maineult, C. Sirtori, R. Colombelli, H. Beere, and D. Ritchie, “Phase-locking of a 2.7-THz quantum cascade laser to a mode-locked erbium-doped fibre laser,” Nat. Photonics4(9), 636–640 (2010). [CrossRef]
• P. Gaal, M. B. Raschke, K. Reimann, and M. Woerner, “Measuring optical frequencies in the 0–40 THz range with non-synchronized electro–optic sampling,” Nat. Photonics1(10), 577–580 (2007). [CrossRef]

Nature

• Th. Udem, R. Holzwarth, and T. W. Hänsch, “Optical frequency metrology,” Nature416(6877), 233–237 (2002). [CrossRef] [PubMed]

Opt. Express

• P. Malara, P. Maddaloni, G. Gagliardi, and P. De Natale, “Absolute frequency measurement of molecular transitions by a direct link to a comb generated around 3-microm,” Opt. Express16(11), 8242–8249 (2008). [CrossRef] [PubMed]
• J. Jiang, A. Onae, H. Matsumoto, and F. L. Hong, “Frequency measurement of acetylene-stabilized lasers using a femtosecond optical comb without carrier-envelope offset frequency control,” Opt. Express13(6), 1958–1965 (2005). [CrossRef] [PubMed]

Opt. Lett.

• C. Erny, K. Moutzouris, J. Biegert, D. Kühlke, F. Adler, A. Leitenstorfer, and U. Keller, “Mid-infrared difference-frequency generation of ultrashort pulses tunable between 3.2 and 4.8 microm from a compact fiber source,” Opt. Lett.32(9), 1138–1140 (2007). [CrossRef] [PubMed]
• A. Gambetta, R. Ramponi, and M. Marangoni, “Mid-infrared optical combs from a compact amplified Er-doped fiber oscillator,” Opt. Lett.33(22), 2671–2673 (2008). [CrossRef] [PubMed]
• S. Bartalini, P. Cancio, G. Giusfredi, D. Mazzotti, P. De Natale, S. Borri, I. Galli, T. Leveque, and L. Gianfrani, “Frequency-comb-referenced quantum-cascade laser at 4.4 microm,” Opt. Lett.32(8), 988–990 (2007). [CrossRef] [PubMed]
• M. Zimmermann, C. Gohle, R. Holzwarth, Th. Udem, and T. W. Hansch, “Optical clockwork with an offset-free difference-frequency comb: accuracy of sum- and difference-frequency generation,” Opt. Lett.29(3), 310–312 (2004). [CrossRef] [PubMed]
• S. M. Foreman, A. Marian, J. Ye, E. A. Petrukhin, M. A. Gubin, O. D. Mücke, F. N. C. Wong, E. P. Ippen, and F. X. Kärtner, “Demonstration of a HeNe/CH4-based optical molecular clock,” Opt. Lett.30(5), 570–572 (2005). [CrossRef] [PubMed]
• A. Amy-Klein, A. Goncharov, M. Guinet, C. Daussy, O. Lopez, A. Shelkovnikov, and C. Chardonnet, “Absolute frequency measurement of a SF6 two-photon line by use of a femtosecond optical comb and sum-frequency generation,” Opt. Lett.30(24), 3320–3322 (2005). [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]
• F. Adler, A. Sell, F. Sotier, R. Huber, and A. Leitenstorfer, “Attosecond relative timing jitter and 13 fs tunable pulses from a two-branch Er:fiber laser,” Opt. Lett.32(24), 3504–3506 (2007). [CrossRef] [PubMed]
• F. Tauser, F. Adler, and A. Leitenstorfer, “Widely tunable sub-30-fs pulses from a compact erbium-doped fiber source,” Opt. Lett.29(5), 516–518 (2004). [CrossRef] [PubMed]
• A. Castrillo, E. De Tommasi, L. Gianfrani, L. Sirigu, and J. Faist, “Doppler-free saturated-absorption spectroscopy of CO2 at 4.3 microm by means of a distributed feedback quantum cascade laser,” Opt. Lett.31(20), 3040–3042 (2006). [CrossRef] [PubMed]

Phys. Rev. Lett.

• S. Bartalini, S. Borri, P. Cancio, A. Castrillo, I. Galli, G. Giusfredi, D. Mazzotti, L. Gianfrani, and P. De Natale, “Observing the intrinsic linewidth of a quantum-cascade laser: beyond the Schawlow-Townes limit,” Phys. Rev. Lett.104(8), 083904 (2010). [CrossRef] [PubMed]

Science

• J. Faist, F. Capasso, D. L. Sivco, C. Sirtori, A. L. Hutchinson, and A. Y. Cho, “Quantum cascade laser,” Science264(5158), 553–556 (1994). [CrossRef] [PubMed]
• M. Beck, D. Hofstetter, T. Aellen, J. Faist, U. Oesterle, M. Ilegems, E. Gini, and H. Melchior, “Continuous Wave Operation of a Mid-Infrared Semiconductor Laser at Room Temperature,” Science295(5553), 301–305 (2002). [CrossRef] [PubMed]
• 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,” Science288(5466), 635–640 (2000). [CrossRef] [PubMed]

Semicond. Sci. Technol.

• A. Hugi, R. Maulini, and J. Faist, “External cavity quantum cascade laser,” Semicond. Sci. Technol.25(8), 083001 (2010). [CrossRef]

Other

• T. A. Johnson and S. A. Diddams, “Mid-IR Frequency Comb Upconversion Spectroscopy”, in Conference on Lasers and Electro-Optics, OSA Technical Digest (CD) (Optical Society of America, 2010), paper CPDB11.

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