The distribution and the comparison of an ultra-stable optical frequency and accurate time using optical fibres have been greatly improved in the last ten years. The frequency stability and accuracy of optical links surpass well-established methods u
sing the global navigation satellite system and geostationary satellites. In this paper, we present a review of the methods and the results obtained. We show that public telecommunication network carrying Internet data can be used to compare and distribute ultra-stable metrological signals over long distances. This novel technique paves the way for the deployment of a national and continental ultra-stable metrological optical network.
Accurate molecular spectroscopy in the mid-infrared region allows precision measurements of fundamental constants. For instance, measuring the linewidth of an isolated Doppler-broadened absorption line of ammonia around 10 $mu$m enables a determinati
on of the Boltzmann constant k B. We report on our latest measurements. By fitting this lineshape to several models which include Dicke narrowing or speed-dependent collisional effects, we find that a determination of k B with an uncertainty of a few ppm is reachable. This is comparable to the best current uncertainty obtained using acoustic methods and would make a significant contribution to any new value of k B determined by the CODATA. Furthermore, having multiple independent measurements at these accuracies opens the possibility of defining the kelvin by fixing k B, an exciting prospect considering the upcoming redefinition of the International System of Units.
A theoretical model of the influence of detection bandwidth properties on observed line shapes in laser absorption spectroscopy is described. The model predicts artificial frequency shifts, extra broadenings and line asymmetries which must be taken i
nto account in order to obtain accurate central frequencies and other spectroscopic parameters. This reveals sources of systematic effects most probably underestimated so far potentially affecting spectroscopic measurements. This may impact many fields of research, from atmospheric and interstellar physics to precision spectroscopic measurements devoted to metrological applications, tests of quantum electrodynamics or other fundamental laws of nature. Our theoretical model is validated by linear absorption experiments performed on H2O and NH3 molecular lines recorded by precision laser spectroscopy in two distinct spectral regions, near- and mid-infrared. Possible means of recovering original line shape parameters or experimental conditions under which the detection bandwidth has a negligible impact, given a targeted accuracy, are proposed. Particular emphasis is put on the detection bandwidth adjustments required to use such high-quality molecular spectra for a spectroscopic determination of the Boltzmann constant at the 1 ppm level of accuracy.
We report the coherent phase-locking of a quantum cascade laser (QCL) at 10-$mu$m to the secondary frequency standard of this spectral region, a CO2 laser stabilized on a saturated absorption line of OsO4. The stability and accuracy of the standard a
re transferred to the QCL resulting in a line width of the order of 10 Hz, and leading to our knowledge to the narrowest QCL to date. The locked QCL is then used to perform absorption spectroscopy spanning 6 GHz of NH3 and methyltrioxorhenium, two species of interest for applications in precision measurements.
To date no experiment has reached the level of sensitivity required to observe weak nuclear force induced parity violation (PV) energy differences in chiral molecules. In this paper, we present the approach, adopted at Laboratoire de Physique des Las
ers (LPL), to measure frequency differences in the vibrational spectrum of enantiomers. We review different spectroscopic methods developed at LPL leading to the highest resolutions, as well as 20 years of CO2 laser stabilization work enabling such precise measurements. After a first attempt to observe PV vibrational frequency shifts using sub-Doppler saturated absorption spectroscopy in a cell, we are currently aiming at an experiment based on Doppler-free two-photon Ramsey interferometry on a supersonic beam. We report on our latest progress towards observing PV with chiral organo-metallic complexes containing a heavy rhenium atom.
We report on our on-going effort to measure the Boltzmann constant, kB, using the Doppler Broadening Technique. The main systematic effects affecting the measurement are discussed. A revised error budget is presented in which the global uncertainty o
n systematic effects is reduced to 2.3 ppm. This corresponds to a reduction of more than one order of magnitude compared to our previous Boltzmann constant measurement. Means to reach a determination of kB at the part per million accuracy level are outlined.
We present a new method for accurate mid-infrared frequency measurements and stabilization to a near-infrared ultra-stable frequency reference, transmitted with a long-distance fibre link and continuously monitored against state-of-the-art atomic fou
ntain clocks. As a first application, we measure the frequency of an OsO4 rovibrational molecular line around 10 $mu$m with a state-of-the-art uncertainty of 8x10-13. We also demonstrate the frequency stabilization of a mid-infrared laser with fractional stability better than 4x10-14 at 1 s averaging time and a line-width below 17 Hz. This new stabilization scheme gives us the ability to transfer frequency stability in the range of 10-15 or even better, currently accessible in the near-infrared or in the visible, to mid-infrared lasers in a wide frequency range.
We have built a frequency chain which enables to measure the absolute frequency of a laser emitting in the 28-31 THz frequency range and stabilized onto a molecular absorption line. The set-up uses an optical frequency comb and an ultrastable 1.55 $m
u$m frequency reference signal, transferred from LNE-SYRTE to LPL through an optical link. We are now progressing towards the stabilization of the mid-IR laser via the frequency comb and the extension of this technique to quantum cascade lasers. Such a development is very challenging for ultrahigh resolution molecular spectroscopy and fundamental tests of physics with molecules.
In this paper we present an accurate analysis of the shape of an isolated rovibrational ammonia line from the strong nu2 band around 10 $mu$m, recorded by laser absorption spectroscopy. Experimental spectra obtained under controlled temperature and p
ressure, are confronted to various models that take into account Dicke narrowing or speed-dependent effects. Our results show clear evidence for speed-dependent broadening and shifting, which had never been demonstrated so far in NH3. Accurate lineshape parameters of the nu2 saQ(6,3) line are obtained. Our current project aiming at measuring the Boltzmann constant, kB, by laser spectroscopy will straight away benefit from such knowledge. We anticipate that a first optical determination of kB with a competitive uncertainty of a few ppm is now reachable.
In this paper, we present significant progress performed on an experiment dedicated to the determination of the Boltzmann constant, k, by accurately measuring the Doppler absorption profile of a line in a gas of ammonia at thermal equilibrium. This o
ptical method based on the first principles of statistical mechanics is an alternative to the acoustical method which has led to the unique determination of k published by the CODATA with a relative accuracy of 1.7 ppm. We report on the first measurement of the Boltzmann constant by laser spectroscopy with a statistical uncertainty below 10 ppm, more specifically 6.4 ppm. This progress results from improvements in the detection method and in the statistical treatment of the data. In addition, we have recorded the hyperfine structure of the probed saQ(6,3) rovibrational line of ammonia by saturation spectroscopy and thus determine very precisely the induced 4.36 (2) ppm broadening of the absorption linewidth. We also show that, in our well chosen experimental conditions, saturation effects have a negligible impact on the linewidth. Finally, we draw the route to future developments for an absolute determination of with an accuracy of a few ppm.
