Olivier Lopez

Optical clocks provide ultraprecise frequency references that are vital for international metrology as well as for tests of fundamental physics. To investigate the level of agreement between different clocks, we simultaneously measured the frequency ratios between ten optical clocks in six different countries, using fiber and satellite links. This is the largest coordinated comparison to date, from which we present a subset of 38 optical frequency ratios and an evaluation of the correlations between them. Four ratios were measured directly for the first time to our knowledge, while others had significantly lower uncertainties than previously achieved, supporting the advance toward a redefinition of the second and the use of optical standards for international time scales.

Using a mid-infrared quantum cascade laser and wavelength modulation absorption spectroscopy, we measure the frequencies of ro-vibrational transitions of N₂O in the 17 µm region with uncertainties below 5 MHz. These lines, corresponding to the bending mode of the molecule, can be used for calibration of spectrometers in this spectral region. We present a model for the lineshapes of absorption features in wavelength modulation spectroscopy that takes into account Doppler broadening, collisional broadening, saturation of the absorption, and lineshape distortion due to frequency and intensity modulation. Combining our data with previous measurements, we provide a set of spectroscopic parameters for several vibrational states of N₂O. The lines measured here fall in the same spectral region as a mid-infrared frequency reference that we are currently developing using trapped, ultracold molecules. With such a frequency reference, the spectroscopic methods demonstrated here have the potential to improve frequency calibration in this part of the spectrum.

We report room temperature heterodyne detection of a quantum cascade laser beaten with a local oscillator on a unipolar quantum photodetector in two different atmospheric windows, at 4.8 $μ$m and 9 $μ$m. A noise equivalent power of few pW is measured by employing an active stabilization technique in which the local oscillator and the signal are locked in phase. The measured heterodyne noise equivalent power is six orders of magnitude lower than that obtained with direct detection.

We report the upgrade and operation of a frequency-comb-assisted high-resolution mid-infrared molecular spectrometer, allowing us to combine high spectral purity, International System of Units (SI)-traceability, wide tunability, and high sensitivity. An optical frequency comb is used to transfer the spectral purity of a SI-traceable 1.54 μm metrology-grade frequency reference to a 10.3 μm quantum cascade laser (QCL). The near-infrared reference is operated at the French time/frequency metrology institute, calibrated there to primary frequency standards, and transferred to Laboratoire de Physique des Lasers via the REFIMEVE fiber network. The QCL exhibits a linewidth of δν ∼ 0.1 Hz and a sub-10−15 relative frequency stability from 0.1 to 10 s, and its frequency is traceable to the SI with a total relative uncertainty better than 4 × 10−14 after 1 s averaging time. We have developed the instrumentation allowing comb modes to be continuously tuned over 9 GHz, resulting in a QCL of record spectral purity uninterruptedly tunable at the precision of the reference over an unprecedented span of Δν = 1.4 GHz. We have used our apparatus to conduct sub-Doppler spectroscopy of methanol in a multi-pass cell, demonstrating state-of-the-art frequency uncertainties down to the few kilohertz level (∼10−10 in relative value). We have observed weak intensity resonances unreported so far, resolved subtle doublets never seen before, and brought to light discrepancies with HITRAN. This demonstrates the potential of our apparatus for probing subtle internal molecular processes, building accurate spectroscopic models of polyatomic molecules of atmospheric or astrophysical interest, and carrying out precise spectroscopic tests of fundamental physics.

We report room temperature heterodyne detection of a quantum cascade laser beaten with a local oscillator on a unipolar quantum photodetector in two different atmospheric windows, at 4.8 µm and 9 µm. A noise equivalent power of few pW is measured by employing an active stabilization technique in which the local oscillator and the signal are locked in phase. The measured heterodyne noise equivalent power is six orders of magnitude lower than that obtained with direct detection.

Phase modulation is demonstrated in a quantum Stark effect modulator designed to operate in the mid-infrared at wavelength around 10 µm. Both phase and amplitude modulation are simultaneously resolved through the measurement of the heterodyne signal arising from the beating of a quantum cascade laser with a highly stabilized frequency comb. The highest measured phase shift is more than 5 degrees with an associated intensity modulation of 5 %. The experimental results are in full agreement with our model in which the complex susceptibility is precisely described considering the linear voltage dependent Stark shift of the optical resonance.

A continuous-wave Fabry–Pérot quantum cascade laser (QCL) emitting at 8.1 μm operating in the single mode regime has been coherently phase locked to a turn-key low-noise commercial mid-Infrared (mid-IR) optical frequency comb. The stability of the comb used as a reference is transferred to the QCL resulting in an integrated residual phase error of 0.4 rad. The laser linewidth is narrowed by more than two orders of magnitude reaching sub-kHz level at 1 ms observation time, limited by the spectral purity of the mid-IR comb. Our experiment is an important step toward the development of both powerful and metrology-grade QCLs and fully stabilized QCL frequency comb and opens perspectives for precision measurements and frequency metrology in the mid-IR.

Aiming at delivering a highly available service, the French national optical fiber link network is run mostly unmanned and automatically, with the help of a global supervision. However, at a year scale, missing data are seemingly unavoidable. Here, we present a first study of the uncertainty of coherent fiber links with missing data. We present the tools to assess statistical properties for processes which are not strictly stationary, and a simulation of optical fiber links depending only on a handful of parameters. We show how missing data affects the phase-coherent optical fiber links, and how to mitigate the issue with a fill-in procedure that preserves the statistical properties. We apply the method for a 5 years-long data set of a 1410 km long fiber link. Second, we apply the method to the case of optical clock comparisons, where the downtimes of the optical clocks degrade the coherence of the links. We show that our methodology of processing the missing data is robust and converges to consistent mean values, even with very low uptimes. We present an offset and uncertainty contribution from the French fiber network of 2.4 (9.0) × 10⁻²⁰, that is an improvement by a factor 5 as compared to a processing without taking the effect of missing data into account.

We present an experimental investigation of the stability limits specific to optical frequency standards using fiber optic architecture and semiconductor lasers. A compact setup composed of a semiconductor laser frequency-locked onto an acetylene transition detected in saturated absorption has been implemented using only fiber optic components. Fiber optic technology allows compact and reliable solutions for various applications. However, for high sensitivity and stability applications such as metrology, residual reflections induced by optical index inhomogeneities in connectors and fiber-coupled components leading to spurious interference significantly limit performance. We have examined the origin of the interference fringes superimposed on the detected signal and the limitations they cause to the frequency stability of the reference. The effects of temperature and beam power fluctuations are also examined. Our results show that the frequency stability is limited in the 10 − 13 range by the effect of interference fringes due to use of fiber components.

Fundamental limits of fiber link are set by non-reciprocal effects that violate the hypothesis of equality between forward and backward path. Non-reciprocal noise arises technically from the set-up asymmetry, and fundamentally by the Sagnac effect when the fiber link encloses a non-zero area. As a pre-requisite for observation of Sagnac effect in fiber links, we present a study on phase noise and frequency stability contributions affecting coherent optical frequency transfer in bi-directional fiber links. Both technical and fundamental limitations of Two-Way optical frequency transfer are discussed. Our model predicts and our experiments substantially verify that the dominant noise mechanism at low Fourier frequencies is the polarization asymmetry induced by the temperature and relative humidity variations impacted on fiber links. The flicker noise floor due to the non-reciprocal noise arising from polarization mode dispersion is evidenced for the first time. We perform a post-processing approach which enables us to remove this polarization noise, improve the long-term stability and remove a frequency bias. We evaluate the uncertainty contributions of all the effects discussed for our 50 km spooled fiber link, dominated by its non-reciprocal noise induced by polarization mode dispersion with uncertainty of 1.9( ± 0.8)( ± 1.2) × 10⁻²⁰. After correction, the linear drift of the residual phase is as low as 27 yoctosecond/s, leading to an uncertainty of the frequency transfer of 2.6 ( ± 39) × 10⁻²², confirming its potential for searching for more fundamental effects such as Sagnac effect or transient frequency variation due to dark matter.