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We present a brief review of our progress towards measuring parity violation in heavy-metal chiral complexes using mid-infrared Ramsey interferometry. We discuss our progress addressing the main challenges, including the development of buffer-gas sources of slow, cold polyatomic molecules, and the frequency-stabilisation of quantum cascade lasers calibrated using primary frequency standards. We report investigations on achiral test species of which promising chiral derivatives have been synthesized.

We carried out a 26-day comparison of five simultaneously operated optical clocks and six atomic fountain clocks located at INRIM, LNE-SYRTE, NPL and PTB by using two satellite-based frequency comparison techniques: broadband Two-Way Satellite Time and Frequency Transfer (TWSTFT) and Global Positioning System Precise Point Positioning (GPS PPP). With an enhanced statistical analysis procedure taking into account correlations and gaps in the measurement data, combined overall uncertainties in the range of $1.8 \times 10^{-16}$ to $3.5 \times 10^{-16}$ for the optical clock comparisons were found. The comparison of the fountain clocks yields results with a maximum relative frequency difference of $6.9 \times 10^{-16}$, and combined overall uncertainties in the range of $4.8 \times 10^{-16}$ to $7.7 \times 10^{-16}$.

There is an increasing demand for precise molecular spectroscopy, in particular in the mid-infrared fingerprint window that hosts a considerable number of vibrational signatures, whether it be for modeling our atmosphere, interpreting astrophysical spectra or testing fundamental physics. We present a high-resolution mid-infrared spectrometer traceable to primary frequency standards. It combines a widely tunable ultra-narrow Quantum Cascade Laser (QCL), an optical frequency comb and a compact multipass cell. The QCL frequency is stabilized onto a comb controlled with a remote near-infrared ultra-stable laser, transferred through a fiber link. The resulting QCL frequency stability is below 10-15 from 0.1 to 10s and its frequency uncertainty of 4x10-14 is given by the remote frequency standards. Continuous tuning over ~400 MHz is reported. We use the apparatus to perform saturated absorption spectroscopy of methanol in the low-pressure multipass cell and demonstrate a statistical uncertainty at the kHz level on transition center frequencies, confirming its potential for driving the next generation technology required for precise spectroscopic measurements.

We report on the first comparison of distant caesium fountain primary frequency standards (PFSs) via an optical fiber link. The 1415 km long optical link connects two PFSs at LNE-SYRTE (Laboratoire National de m\'{e}trologie et d'Essais - SYst\`{e}me de R\'{e}f\'{e}rences Temps-Espace) in Paris (France) with two at PTB (Physikalisch-Technische Bundesanstalt) in Braunschweig (Germany). For a long time, these PFSs have been major contributors to accuracy of the International Atomic Time (TAI), with stated accuracies of around $3\times 10^{-16}$. They have also been the references for a number of absolute measurements of clock transition frequencies in various optical frequency standards in view of a future redefinition of the second. The phase coherent optical frequency transfer via a stabilized telecom fiber link enables far better resolution than any other means of frequency transfer based on satellite links. The agreement for each pair of distant fountains compared is well within the combined uncertainty of a few 10$^{-16}$ for all the comparisons, which fully supports the stated PFSs' uncertainties. The comparison also includes a rubidium fountain frequency standard participating in the steering of TAI and enables a new absolute determination of the $^{87}$Rb ground state hyperfine transition frequency with an uncertainty of $3.1\times 10^{-16}$. This paper is dedicated to the memory of Andr\'{e} Clairon, who passed away on the 24$^{th}$ of December 2015, for his pioneering and long-lasting efforts in atomic fountains. He also pioneered optical links from as early as 1997.

We use six years of accurate hyperfine frequency comparison data of the dual rubidium and caesium cold atom fountain FO2 at LNE-SYRTE to search for a massive scalar dark matter candidate. Such a scalar field can induce harmonic variations of the fine structure constant, of the mass of fermions and of the quantum chromodynamic mass scale, which will directly impact the rubidium/caesium hyperfine transition frequency ratio. We find no signal consistent with a scalar dark matter candidate but provide improved constraints on the coupling of the putative scalar field to standard matter. Our limits are complementary to previous results that were only sensitive to the fine structure constant, and improve them by more than an order of magnitude when only a coupling to electromagnetism is assumed., Comment: 5 pages (+2 pages of supplemental material), 4 figures, version accepted for publication in Phys. Rev. Letters

In this paper we report the evaluation of an optical lattice clock based on neutral mercury down to a relative uncertainty of $1.7\times 10^{-16}$. Comparing this characterized frequency standard to a Cs atomic fountain we determine the absolute frequency of the $^1S_0 \rightarrow \phantom{}^3P_0$ transition of $^{199}$Hg as $\nu_{\mathrm{Hg}} = 1 128\,575\,290\,808\,154.62\,$Hz $\pm\,0.19\,$Hz (statistical) $\pm\,0.38\,$Hz (systematic), limited solely by the realization of the SI second. Furthermore, by comparing the mercury optical lattice clock to a Rb atomic fountain, we determine for the first time to our knowledge the ratio between the $^{199}$Hg clock transition and the $^{87}$Rb ground state hyperfine transition. Finally we present a direct optical to optical measurement of the $^{199}$Hg/$^{87}$Sr frequency ratio. The obtained value of $\nu_{\mathrm{Hg}}/\nu_{\mathrm{Sr}}=2.629\,314\,209\,898\,909\,15$ with a fractional uncertainty of $1.8\times10^{-16}$ is in excellent agreement with the same measurement obtained by Yamanaka et al. (arXiv:1503.07941). This makes this frequency ratio one of the few physical quantities agreed upon by different laboratories to this level of uncertainty. Frequency ratio measurements of the kind of those reported in this paper have a strong impact for frequency metrology but also for fundamental physics as they can be used to monitor putative variations of fundamental constants., Comment: 23 pages, 12 figures, updated version including journal reference

Leveraging the unrivaled performance of optical clocks in applications in fundamental physics beyond the standard model, in geo-sciences, and in astronomy requires comparing the frequency of distant optical clocks truthfully. Meeting this requirement, we report on the first comparison and agreement of fully independent optical clocks separated by 700 km being only limited by the uncertainties of the clocks themselves. This is achieved by a phase-coherent optical frequency transfer via a 1415 km long telecom fiber link that enables substantially better precision than classical means of frequency transfer. The fractional precision in comparing the optical clocks of three parts in $10^{17}$ was reached after only 1000 s averaging time, which is already 10 times better and more than four orders of magnitude faster than with any other existing frequency transfer method. The capability of performing high resolution international clock comparisons paves the way for a redefinition of the unit of time and an all-optical dissemination of the SI-second., Comment: 14 pages, 3 figures, 1 table

In this article, we report on the work done with the LNE-SYRTE atomic clock ensemble during the last 10 years. We cover progress made in atomic fountains and in their application to timekeeping. We also cover the development of optical lattice clocks based on strontium and on mercury. We report on tests of fundamental physical laws made with these highly accurate atomic clocks. We also report on work relevant to a future possible redefinition of the SI second.

The frequencies of three separate Cs fountain clocks and one Rb fountain clock have been compared to various hydrogen masers to search for periodic changes correlated with the changing solar gravitational potential at the Earth and boost with respect to the Cosmic Microwave Background (CMB) rest frame. The data sets span over more than eight years. The main sources of long-term noise in such experiments are the offsets and linear drifts associated with the various H-masers. The drift can vary from nearly immeasurable to as high as 1.3*10^-15 per day. To circumvent these effects we apply a numerical derivative to the data, which significantly reduces the standard error when searching for periodic signals. We determine a standard error for the putative Local Position Invariance (LPI) coefficient with respect to gravity for a Cs-Fountain H-maser comparison of 4.8*10^-6 and 10^-5 for a Rb-Fountain H-maser comparison. From the same data the putative boost LPI coefficients were measured to a precision of up to parts in 10^11 with respect to the CMB rest frame. By combining these boost invariance experiments to a Cryogenic Sapphire Oscillator versus H-maser comparison, independent limits on all nine coefficients of the boost violation vector with respect to fundamental constant invariance (fine structure constant, electron mass and quark mass respectively), were determined to a precision of parts up to 10^10., Comment: accepted for publication in Phys Rev D

Progress in realizing the SI second had multiple technological impacts and enabled to further constraint theoretical models in fundamental physics. Caesium microwave fountains, realizing best the second according to its current definition with a relative uncertainty of 2-4x10^(-16), have already been superseded by atomic clocks referenced to an optical transition, both more stable and more accurate. Are we ready for a new definition of the second? Here we present an important step in this direction: our system of five clocks connects with an unprecedented consistency the optical and the microwave worlds. For the first time, two state-of-the-art strontium optical lattice clocks are proven to agree within their accuracy budget, with a total uncertainty of 1.6x10^(-16). Their comparison with three independent caesium fountains shows a degree of reproducibility henceforth solely limited at the level of 3.1x10^(-16) by the best realizations of the microwave-defined second., Comment: 9 pages, 4 figures, 2 tables

We report the operation of a dual Rb/Cs atomic fountain clock. 133Cs and 87Rb atoms are cooled, launched, and detected simultaneously in LNE-SYRTE's FO2 double fountain. The dual clock operation occurs with no degradation of either the stability or the accuracy. We describe the key features for achieving such a simultaneous operation. We also report on the results of the first Rb/Cs frequency measurement campaign performed with FO2 in this dual atom clock configuration, including a new determination of the absolute 87Rb hyperfine frequency., Comment: 6 pages, 10 figures, 23 references

We demonstrate the use of a fiber-based femtosecond laser locked onto an ultra-stable optical cavity to generate a low-noise microwave reference signal. Comparison with both a liquid Helium cryogenic sapphire oscillator (CSO) and a Ti:Sapphire-based optical frequency comb system exhibit a stability about $3\times10^{-15}$ between 1 s and 10 s. The microwave signal from the fiber system is used to perform Ramsey spectroscopy in a state-of-the-art Cesium fountain clock. The resulting clock system is compared to the CSO and exhibits a stability of $3.5\times10^{-14}\tau^{-1/2}$. Our continuously operated fiber-based system therefore demonstrates its potential to replace the CSO for atomic clocks with high stability in both the optical and microwave domain, most particularly for operational primary frequency standards., Comment: 3 pages, 3 figures

We report on the first absolute transition frequency measurement at the 10^{-15} level with a single, laser-cooled 40Ca+ ion in a linear Paul trap. For this measurement, a frequency comb is referenced to the transportable Cs atomic fountain clock of LNE-SYRTE and is used to measure the S1/2-D5/2 electric-quadrupole transition frequency. After the correction of systematic shifts, the clock transition frequency f_Ca+ = 411 042 129 776 393.2 (1.0) Hz is obtained, which corresponds to a fractional uncertainty within a factor of three of the Cs standard. Future improvements are expected to lead to an uncertainty surpassing the best Cs fountain clocks. In addition, we determine the Lande g-factor of the D5/2 level to be gD5/2=1.2003340(3).

This paper describes advances in microwave frequency standards using laser-cooled atoms at BNM-SYRTE. First, recent improvements of the $^{133}$Cs and $^{87}$Rb atomic fountains are described. Thanks to the routine use of a cryogenic sapphire oscillator as an ultra-stable local frequency reference, a fountain frequency instability of $1.6\times 10^{-14}\tau^{-1/2}$ where $\tau $ is the measurement time in seconds is measured. The second advance is a powerful method to control the frequency shift due to cold collisions. These two advances lead to a frequency stability of $2\times 10^{-16}$ at $50,000s for the first time for primary standards. In addition, these clocks realize the SI second with an accuracy of $7\times 10^{-16}$, one order of magnitude below that of uncooled devices. In a second part, we describe tests of possible variations of fundamental constants using $^{87}$Rb and $^{133}$Cs fountains. Finally we give an update on the cold atom space clock PHARAO developed in collaboration with CNES. This clock is one of the main instruments of the ACES/ESA mission which is scheduled to fly on board the International Space Station in 2008, enabling a new generation of relativity tests., Comment: 30 pages, 11 figures

We have remeasured the absolute $1S$-$2S$ transition frequency $\nu_{\rm {H}}$ in atomic hydrogen. A comparison with the result of the previous measurement performed in 1999 sets a limit of $(-29\pm 57)$ Hz for the drift of $\nu_{\rm {H}}$ with respect to the ground state hyperfine splitting $\nu_{{\rm {Cs}}}$ in $^{133}$Cs. Combining this result with the recently published optical transition frequency in $^{199}$Hg$^+$ against $\nu_{\rm {Cs}}$ and a microwave $^{87}$Rb and $^{133}$Cs clock comparison, we deduce separate limits on $\dot{\alpha}/\alpha = (-0.9\pm 2.9)\times 10^{-15}$ yr$^{-1}$ and the fractional time variation of the ratio of Rb and Cs nuclear magnetic moments $\mu_{\rm {Rb}}/\mu_{\rm {Cs}}$ equal to $(-0.5 \pm 1.7)\times 10^{-15}$ yr$^{-1}$. The latter provides information on the temporal behavior of the constant of strong interaction., Comment: 4 pages, 3 figures, LaTeX

In 2003 we have measured the absolute frequency of the $(1S, F=1, m_F=\pm 1) \leftrightarrow (2S, F'=1, m_F'=\pm 1)$ two-photon transition in atomic hydrogen. We observed a variation of $(-29\pm 57)$ Hz over a 44 months interval separating this measurement from the previous one performed in 1999. We have combined this result with recently published results of optical transition frequency measurement in the $^{199}$Hg$^+$ ion and and comparison between clocks based on $^{87}$Rb and $^{133}$Cs. From this combination we deduce the stringent limits for fractional time variation of the fine structure constant $\partial/{\partial t}(\ln \alpha)=(-0.9\pm 4.2)\times 10^{-15}$ yr$^{-1}$ and for the ratio of $^{87}$Rb and $^{133}$Cs spin magnetic moments $\partial/{\partial t}(\ln[\mu_{\rm {Rb}}/\mu_{\rm {Cs}}])=(0.5\pm 2.1)\times 10^{-15}$ yr$^{-1}$. This is the first precise restriction for the fractional time variation of $\alpha$ made without assumptions about the relative drifts of the constants of electromagnetic, strong and weak interactions., Comment: 18 pages, 10 figures, invited talk

We describe two experimental tests of the Equivalence Principle that are based on frequency measurements between precision oscillators and/or highly accurate atomic frequency standards. Based on comparisons between the hyperfine frequencies of 87Rb and 133Cs in atomic fountains, the first experiment constrains the stability of fundamental constants. The second experiment is based on a comparison between a cryogenic sapphire oscillator and a hydrogen maser. It tests Local Lorentz Invariance. In both cases, we report recent results which improve significantly over previous experiments., Comment: 13 pages, 5 figures

Over five years we have compared the hyperfine frequencies of 133Cs and 87Rb atoms in their electronic ground state using several laser cooled 133Cs and 87Rb atomic fountains with an accuracy of ~10^{-15}. These measurements set a stringent upper bound to a possible fractional time variation of the ratio between the two frequencies : (d/dt)ln(nu_Rb/nu_Cs)=(0.2 +/- 7.0)*10^{-16} yr^{-1} (1 sigma uncertainty). The same limit applies to a possible variation of the quantity (mu_Rb/mu_Cs)*alpha^{-0.44}, which involves the ratio of nuclear magnetic moments and the fine structure constant., Comment: 4 pages, 3 figures, 1 table submitted to Phys. Rev. Lett