Quantum correlation-enhanced dual-comb spectroscopy

Zhuoren Wan; Yuan Chen; Xiuxiu Zhang; Ming Yan; Heping Zeng

doi:10.1038/s41377-025-01891-1

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Quantum correlation-enhanced dual-comb spectroscopy

Original Articles

- Quantum correlation-enhanced dual-comb spectroscopy
- Light: Science & Applications Vol. 14, Issue 9, Pages: 2665-2673(2025)
- Affiliations：
  
  1.State Key Laboratory of Precision Spectroscopy, and Hainan Institute, East China Normal University, Shanghai, China
  2.Chongqing Key Laboratory of Precision Optics, Chongqing Institute of East China Normal University, 401120 Chongqing, China
  3.Hainan Institute of East China Normal University, 572025 Sanya, China
  4.Jinan Institute of Quantum Technology, 250101 Jinan, Shandong, China
- Author bio：
  
  Ming Yan (myan@lps.ecnu.edu.cn)
  Heping Zeng (hpzeng@phy.ecnu.edu.cn)
- Funds：
- DOI：10.1038/s41377-025-01891-1
  CLC：
- Received：18 December 2024，
  
  Revised：2025-04-28，
  
  Accepted：12 May 2025，
  
  Published Online：01 August 2025，
  
  Published：30 September 2025
- Accepted：
Scan QR Code
Wan, Z. R. et al. Quantum correlation-enhanced dual-comb spectroscopy. Light: Science & Applications, 14, 2665-2673 (2025).
DOI：

Wan, Z. R. et al. Quantum correlation-enhanced dual-comb spectroscopy. Light: Science & Applications, 14, 2665-2673 (2025). DOI： 10.1038/s41377-025-01891-1.

摘要

Abstract

Dual-comb spectroscopy (DCS) is a powerful technique for spectroscopic sensing

offering exceptional spectral bandwidth

resolution

precision

and speed. However

its performance is fundamentally limited by quantum noise inherent to coherent-state optical combs. Here

we overcome this barrier by introducing quantum correlation-enhanced DCS using correlated twin combs generated via seeded four-wave mixing. One comb acts as a local oscillator to decode molecular signals

while the twin suppresses shot noise through intensity-difference squeezing

achieving a 2 dB signal-to-noise ratio improvement beyond the shot-noise limit—equivalent to a 2.6× measurement speed enhancement. Notably

when coupled with up-conversion spectroscopy

our technique records comb-line-resolved

high-resolution (7.5 pm) spectra in the critical 3 μm region for molecular fingerprinting. These results bridge quantum optics and frequency comb spectroscopy

offering great potential for trace gas detection

precision metrology

and chemical analysis. Future developments in detector efficiency and nanophotonic integration could further enhance its scalability and impact.

关键词

Keywords

references

Coddington, I., Newbury, N. & Swann, W. Dual-comb spectroscopy. Optica 3 , 414–426 (2016)..

Weichman, M. L. et al. Broadband molecular spectroscopy with optical frequency combs. J. Mol. Spectrosc. 355 , 66–78 (2019)..

Luo, P. L. Long-wave mid-infrared time-resolved dual-comb spectroscopy of short-lived intermediates. Opt. Lett. 45 , 6791–6794 (2020)..

Long, D. A. et al. Nanosecond time-resolved dual-comb absorption spectroscopy. Nat. Photonics 18 , 127–131 (2024)..

Rieker, G. B. et al. Frequency-comb-based remote sensing of greenhouse gases over kilometer air paths. Optica 1 , 290–298 (2014)..

Han, J. J. et al. Dual-comb spectroscopy over a 100 km open-air path. Nat. Photonics 18 , 1195–1202 (2024)..

Cossel, K. C. et al. Open-path dual-comb spectroscopy to an airborne retroreflector. Optica 4 , 724–728 (2017)..

Yan, M. et al. Mid-infrared dual-comb spectroscopy with electro-optic modulators. Light Sci. Appl. 6 , e17076 (2017)..

Ycas, G. et al. High-coherence mid-infrared dual-comb spectroscopy spanning 2.6 to 5.2 μm. Nat. Photonics 12 , 202–208 (2018)..

Muraviev, A. V. et al. Massively parallel sensing of trace molecules and their isotopologues with broadband subharmonic mid-infrared frequency combs. Nat. Photonics 12 , 209–214 (2018)..

Kowligy, A. S. et al. Infrared electric field sampled frequency com b spectroscopy. Sci. Adv. 5 , eaaw8794 (2019)..

Bernhardt, B. et al. Cavity-enhanced dual-comb spectroscopy. Nat. Photonics 4 , 55–57 (2009)..

Hoghooghi, N. et al. Broadband coherent cavity-enhanced dual-comb spectroscopy. Optica 6 , 28–33 (2019)..

Chen, Z., Hänsch, T. W. & Picqué, N. Upconversion mid-infrared dual-comb spectroscopy. Preprint at https://doi.org/10.48550/arXiv.2003.06930 https://doi.org/10.48550/arXiv.2003.06930 (2020).

Wen, Z. Y. et al. Broadband up-conversion mid-infrared time-stretch spectroscopy. Laser Photonics Rev. 18 , 2300630 (2024)..

Sun, B. et al. Single-photon time-stretch infrared spectroscopy. Laser Photonics Rev. 18 , 2301272 (2024)..

Newbury, N. R., Coddington, I. & Swann, W. Sensitivity of coherent dual-comb spectroscopy. Opt. Express 18 , 7929–7945 (2010)..

Caldwell, E. D. et al. The t ime-programmable frequency comb and its use in quantum-limited ranging. Nature 610 , 667–673 (2022)..

Lomsadze, B., Smith, B. C. & Cundiff, S. T. Tri-comb spectroscopy. Nat. Photonics 12 , 676–680 (2018)..

Barik, P. & Pradhan, M. Selectivity in trace gas sensing: recent developments, challenges, and future perspectives. Analyst 147 , 1024–1054 (2022)..

Aasi, J. et al. Enhanced sensitivity of the LIGO gravitational wave detector by using squeezed states of light. Nat. Photonics 7 , 613–619 (2013)..

Casacio, C. A. et al. Quantum-enhanced nonlinear microscopy. Nature 594 , 201–206 (2021)..

Polzik, E. S., Carri, J. & Kimble, H. J. Atomic spectroscopy with squeezed light for sensitivity beyond the vacuum-state limit. Appl. Phys. B 55 , 279–290(1992)..

Polzik, E. S., Carri, J. & Kimble, H. J. Spectroscopy with squeezed light. Phys. Rev. Lett. 68 , 3020–3023 (1992)..

Li, Y. Q., Guzun, D. & Xiao, M. Sub-shot-noise-limited optical heterodyne detection using an amplitude-squeezed local oscillator. Phys. Rev. Lett. 82 , 5225–5228 (1999)..

Lordi, N. et al. Quantum theory of temporally mismatched homodyne measurements with applications to optical-frequency-comb metrology. Phys. Rev. A 109 , 033722 (2024)..

Shi, H. W. et al. Entanglement-enhanced dual-comb spectroscopy. npj Quantum Inf. 9 , 91 (2023)..

Herman, D. I. et al. Squeezed dual-comb spectroscopy. Science 387 , 653–658 (2025)..

Zhang, D. et al. Enhanced intensity-difference squeezing via energy-level modulations in hot atomic media. Phys. Rev. A 96 , 043847 (2017)..

Rarity, J. G. et al. Photonic crystal fiber source of correlated photon pairs. Opt. Express 13 , 534–544 (2005)..

Sharping, J. E., Fiorentino, M. & Kumar, P. Observation of twin-beam-type quantum correlation in optical fiber. Opt. Lett. 26 , 367–369 (2001)..

Guo, X. S. et al. Multimode theory of pulsed-twin-beam generation using a high-gain fiber-optical parametric amplifier. Phys. Rev. A 88 , 023841 (2013)..

Liu, S. S., Lou, Y. B. & Jing, J. T. Interference-induced quantum squeezing enhancement in a two-beam phase-sensitive amplifier. Phys. Rev. Lett. 123 , 113602 (2019)..

Schnabel, R. Squeezed states of light and their applications in laser interferometers. Phys. Rep. 684 , 1–51 (2017)..

Anisimov, P. M. et al. Quantum metrology with two-mode squeezed vacuum: parity detection beats the heisenberg limit. Phys. Rev. Lett. 104 , 103602 (2010)..

Lawrie, B. J. et al. Quantum sensing with squeezed light. ACS Photonics 6 , 1307–1318 (2019)..

Boyer,V. et al. Entangled images from four-wave mixing. Science 321 , 544–547 (2008)..

Ideguchi, T. et al. Coherent Raman spectro-imaging with laser frequency combs. Nature 502 , 355–358 (2013)..

Jasperse, M., Turner, L. D. & Scholten, R. E. Relative intensity squeezing by four-wave mixing with loss: an analytic model and experimental diagnostic. Opt. Express 19 , 3765–3774 (2011)..

Deschênes, J. D. & Genest, J. Heterodyne beats between a continuous-wave laser and a frequency comb beyond the shot-noise limit of a single comb mode. Phys. Rev. A 87 , 023802 (2013)..

Walsh, M., Guay, P. & Genest, J. Unlocking a lower shot noise limit in dual-comb interferometry. APL Photonics 8 , 071302 (2023)..

Millot, G. et al. Frequency-agile dual-comb spectroscopy. Nat. Photonics 10 , 27–30 (2016)..

Yang, Z. J. et al. A squeezed quantum microcomb on a chip. Nat. Commun. 12 , 4781 (2021)..

Guay, P. et al. Linear dual-comb interferometry at high power levels. Opt. Express 31 , 4393–4404 (2023)..

Lin, Q. & Agrawal, G. P. Silicon waveguides for creating quantum-correlated photon pairs. Opt. Lett. 31 , 3140–3142 (2006)..

Dutt, A. et al. On-chip optical squeezing. Phys. Rev. Appl. 3 , 044005 (2015)..

Zhang, Y. et al. Squeezed light from a nanophotonic molecule. Nat. Commun. 12 , 2233 (2021)..

Ren, X. Y. et al. Dual-comb optomechanical spectroscopy. Nat. Commun. 14 , 5037 (2023)..

Thorpe, M. J. et al. Cavity-enhanced optical frequency comb spectroscopy: application to human breath analysis. Opt. Express 16 , 2387–2397 (2008)..

Coddington, I. et al. Rapid and precise absolute distance measurements at long range. Nat. Photonics 3 , 351–356 (2009)..

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