Comb-locked frequency-swept synthesizer for high precision broadband spectroscopy

Frequency combs have made optical metrology accessible to hundreds of laboratories worldwide and they have set new benchmarks in multi-species trace gas sensing for environmental, industrial and medical applications. However, current comb spectrometers privilege either frequency precision and sensitivity through interposition of a cw probe laser with limited tuning range, or spectral coverage and measurement time using the comb itself as an ultra-broadband probe. We overcome this restriction by introducing a comb-locked frequency-swept optical synthesizer that allows a continuous-wave laser to be swept in seconds over spectral ranges of several terahertz while remaining phase locked to an underlying frequency comb. This offers a unique degree of versatility, as the synthesizer can be either repeatedly scanned over a single absorption line to achieve ultimate precision and sensitivity, or swept in seconds over an entire rovibrational band to capture multiple species. The spectrometer enables us to determine line center frequencies with an absolute uncertainty of 30 kHz and at the same time to collect absorption spectra over more than 3 THz with state-of-the-art sensitivity of a few 10 −10  cm −1 . Beyond precision broadband spectroscopy, the proposed synthesizer is an extremely promising tool to force a breakthrough in terahertz metrology and coherent laser ranging.

[1]  Jun Ye,et al.  CAVITY-ENHANCED OPTICAL FREQUENCY COMB SPECTROSCOPY , 2009 .

[2]  P. Pfeiffer,et al.  Comb-calibrated frequency sweeping interferometry for absolute distance and vibration measurement. , 2019, Optics letters.

[3]  Thomas Puppe,et al.  Phase-predictable tuning of single-frequency optical synthesizers. , 2014, Optics letters.

[4]  Julien Mandon,et al.  Fourier transform spectroscopy with a laser frequency comb , 2009 .

[5]  J. Hodges,et al.  Comb-linked, cavity ring-down spectroscopy for measurements of molecular transition frequencies at the kHz-level. , 2013, The Journal of chemical physics.

[6]  P. Laporta,et al.  Conjugating precision and acquisition time in a Doppler broadening regime by interleaved frequency-agile rapid-scanning cavity ring-down spectroscopy. , 2017, The Journal of chemical physics.

[7]  A. Luiten,et al.  Accurate lineshape spectroscopy and the Boltzmann constant , 2015, Nature Communications.

[8]  Ming Yan,et al.  Mid-infrared dual-comb spectroscopy with electro-optic modulators , 2017, Light, science & applications.

[9]  I. Coddington,et al.  Coherent multiheterodyne spectroscopy using stabilized optical frequency combs. , 2007, Physical review letters.

[10]  Richard T. White,et al.  A quantitative mode-resolved frequency comb spectrometer. , 2015, Optics express.

[11]  Kevin F. Lee,et al.  Self-referenced, accurate and sensitive optical frequency comb spectroscopy with a virtually imaged phased array spectrometer. , 2016, Optics letters.

[12]  Amanda S. Makowiecki,et al.  Broadband coherent cavity-enhanced dual-comb spectroscopy , 2019, Optica.

[13]  Jun Ye,et al.  Quantum-noise-limited optical frequency comb spectroscopy. , 2011, Physical review letters.

[14]  W. DiNatale,et al.  Generation and detection of coherent terahertz waves using two photomixers , 1998 .

[15]  H Matsumoto,et al.  Phase-locked widely tunable optical single-frequency generator based on a femtosecond comb. , 2005, Optics letters.

[16]  J. Hodges,et al.  Frequency-agile, rapid scanning spectroscopy , 2013, Nature Photonics.

[17]  Markus Brehm,et al.  Frequency-comb infrared spectrometer for rapid, remote chemical sensing. , 2005, Optics express.

[18]  Jean-Daniel Deschênes,et al.  Continuous real-time correction and averaging for frequency comb interferometry. , 2012, Optics express.

[19]  P. Laporta,et al.  Scanning micro-resonator direct-comb absolute spectroscopy , 2016, Scientific Reports.

[20]  J. Komasa,et al.  Toward a Determination of the Proton-Electron Mass Ratio from the Lamb-Dip Measurement of HD. , 2017, Physical review letters.

[21]  Ming Yan,et al.  A phase-stable dual-comb interferometer , 2018, Nature Communications.

[22]  Daniele Romanini,et al.  Introduction to Cavity Enhanced Absorption Spectroscopy , 2014 .

[23]  T. Hänsch,et al.  Adaptive real-time dual-comb spectroscopy , 2012, Nature Communications.

[24]  Esther Baumann,et al.  High-coherence mid-infrared dual-comb spectroscopy spanning 2.6 to 5.2 μm , 2017, 1709.07105.

[25]  F. Thibault,et al.  Accurate deuterium spectroscopy for fundamental studies , 2018, Journal of Quantitative Spectroscopy and Radiative Transfer.

[26]  Kevin F. Lee,et al.  Rovibrational quantum state resolution of the C60 fullerene , 2018, Science.

[27]  K. Eikema,et al.  SUB-DOPPLER FREQUENCY METROLOGY IN HD FOR TEST OF FUNDAMENTAL PHYSICS , 2018, Proceedings of the 73rd International Symposium on Molecular Spectroscopy.

[28]  Jun Ye,et al.  Mid-Infrared Time-Resolved Frequency Comb Spectroscopy of Transient Free Radicals. , 2014, The journal of physical chemistry letters.

[29]  Thomas Udem,et al.  Cavity-enhanced dual-comb spectroscopy , 2009, 0908.1928.

[30]  P. Laporta,et al.  Comb-locked cavity ring-down spectrometer. , 2015, The Journal of chemical physics.

[31]  I. Coddington,et al.  Characterizing Fast Arbitrary CW Waveforms With 1500 THz/s Instantaneous Chirps , 2012, IEEE Journal of Selected Topics in Quantum Electronics.

[32]  E. R. Polovtseva,et al.  The HITRAN2012 molecular spectroscopic database , 2013 .

[33]  Jun Ye,et al.  Continuously tunable, precise, single frequency optical signal generator. , 2002, Optics express.

[34]  M. Gorodetsky,et al.  Frequency comb assisted diode laser spectroscopy for measurement of microcavity dispersion , 2009, 0907.0143.

[35]  A. John Alcock,et al.  Accurate absolute reference frequencies from 1511 to 1545 nm of the ν1+ν3 band of 12 C2H2 determined with laser frequency comb interval measurements , 2006 .

[36]  Piotr Maslowski,et al.  Optical frequency comb Fourier transform spectroscopy with sub-nominal resolution and precision beyond the Voigt profile , 2018 .

[37]  Paul R. Berman,et al.  Speed-dependent collisional width and shift parameters in spectral profiles , 1972 .

[38]  Gang Li,et al.  The HITRAN 2008 molecular spectroscopic database , 2005 .

[39]  D. Romanini,et al.  Optical feedback frequency-stabilized cavity ring-down spectroscopy - Highly coherent near-infrared laser sources and metrological applications in molecular absorption spectroscopy , 2015 .

[40]  Konstantin L. Vodopyanov,et al.  Massively parallel sensing of trace molecules and their isotopologues with broadband subharmonic mid-infrared frequency combs , 2018 .

[41]  A. Foltynowicz,et al.  Cavity-enhanced optical frequency comb spectroscopy in the mid-infrared application to trace detection of hydrogen peroxide , 2012, 1202.1216.

[42]  Esther Baumann,et al.  Fast high-resolution spectroscopy of dynamic continuous-wave laser sources , 2010 .

[43]  Scott A. Diddams,et al.  Molecular fingerprinting with the resolved modes of a femtosecond laser frequency comb , 2007, Nature.

[44]  T. C. Briles,et al.  Optical frequency comb spectroscopy. , 2011, Faraday discussions.

[45]  D. Hurtmans,et al.  Frequency comb-referenced measurements of self- and nitrogen-broadening in the ν1 + ν3 band of acetylene , 2011 .

[46]  K. Eikema,et al.  Sub-Doppler Frequency Metrology in HD for Tests of Fundamental Physics. , 2017, Physical review letters.

[47]  Erik Benkler,et al.  Endless frequency shifting of optical frequency comb lines. , 2013, Optics express.