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This paper gives a detailed account of the analysis underpinning the 2021 update to the list of standard reference frequency values recommended by the International Committee for Weights and Measures (CIPM). This update focused on a subset of atomic transitions that are secondary representations of the second (SRS) or considered as potential SRS. As in previous updates in 2015 and 2017, methods for analysing over-determined data sets were applied to make optimum use of the worldwide body of published clock comparison data. To ensure that these methods were robust, three independent calculations were performed using two different algorithms. The 2021 update differed from previous updates in taking detailed account of correlations among the input data, a step shown to be important in deriving unbiased frequency values and avoiding underestimation of their uncertainties. It also differed in the procedures used to assess input data and to assign uncertainties to the recommended frequency values, with previous practice being adapted to produce a fully consistent output data set consisting of frequency ratio values as well as absolute frequencies. These changes are significant in the context of an anticipated redefinition of the second in terms of an optical transition or transitions, since optical frequency ratio measurements will be critical for verifying the international consistency of optical clocks prior to the redefinition. In the meantime, the reduced uncertainties for optical SRS resulting from this analysis significantly increases the weight that secondary frequency standards based on these transitions can have in the steering of International Atomic Time (TAI)., Comment: 22 pages, 5 figures

This paper outlines the roadmap towards the redefinition of the second, which was recently updated by the CCTF Task Force created by the CCTF in 2020. The main achievements and the open challenges related to the status of the optical frequency standards, their contribution to time scales and UTC, the possibility of their comparison and the knowledge of the Earth's gravitational potential at the necessary level of uncertainty are discussed. In addition, the mandatory criteria to be achieved before redefinition and their current fulfilment level, together with the redefinition options based on a single or on a set of transitions are described., Comment: 26 pages. This paper is based on the work of a CCTF Task Force on the roadmap to the redefinition of the second

The detection of variations of fundamental constants of the Standard Model would provide us with compelling evidence of new physics, and could lift the veil on the nature of dark matter and dark energy. In this work, we discuss how a network of atomic and molecular clocks can be used to look for such variations with unprecedented sensitivity over a wide range of time scales. This is precisely the goal of the recently launched QSNET project: A network of clocks for measuring the stability of fundamental constants. QSNET will include state-of-the-art atomic clocks, but will also develop next-generation molecular and highly charged ion clocks with enhanced sensitivity to variations of fundamental constants. We describe the technological and scientific aims of QSNET and evaluate its expected performance. We show that in the range of parameters probed by QSNET, either we will discover new physics, or we will impose new constraints on violations of fundamental symmetries and a range of theories beyond the Standard Model, including dark matter and dark energy models.

The QSNET consortium is building a UK network of next-generation atomic and molecular clocks that will achieve unprecedented sensitivity in testing variations of the fine structure constant, $\alpha$, and the electron-to-proton mass ratio, $\mu$. This in turn will provide more stringent constraints on a wide range of fundamental and phenomenological theories beyond the Standard Model and on dark matter models.

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 $7.7 \times 10^{-16}$.

We search for transient variations of the fine structure constant using data from a European network of fiber-linked optical atomic clocks. By searching for coherent variations in the recorded clock frequency comparisons across the network, we significantly improve the constraints on transient variations of the fine structure constant. For example, we constrain the variation in alpha to <5*10^-17 for transients of duration 10^3 s. This analysis also presents a possibility to search for dark matter, the mysterious substance hypothesised to explain galaxy dynamics and other astrophysical phenomena that is thought to dominate the matter density of the universe. At the current sensitivity level, we find no evidence for dark matter in the form of topological defects (or, more generally, any macroscopic objects), and we thus place constraints on certain potential couplings between the dark matter and standard model particles, substantially improving upon the existing constraints, particularly for large (>~10^4 km) objects.

Phase compensated optical fiber links enable high accuracy atomic clocks separated by thousands of kilometers to be compared with unprecedented statistical resolution. By searching for a daily variation of the frequency difference between four strontium optical lattice clocks in different locations throughout Europe connected by such links, we improve upon previous tests of time dilation predicted by special relativity. We obtain a constraint on the Robertson--Mansouri--Sexl parameter $|\alpha|\lesssim 1.1 \times10^{-8}$ quantifying a violation of time dilation, thus improving by a factor of around two the best known constraint obtained with Ives--Stilwell type experiments, and by two orders of magnitude the best constraint obtained by comparing atomic clocks. This work is the first of a new generation of tests of fundamental physics using optical clocks and fiber links. As clocks improve, and as fiber links are routinely operated, we expect that the tests initiated in this paper will improve by orders of magnitude in the near future., Comment: 6 pages, 3 figures, published in Phys. Rev. L

We used Precise Point Positioning, a well-established GPS carrier-phase frequency transfer method to perform a direct remote comparison of two optical frequency standards based on single laser-cooled $^{171}$Yb$^+$ ions operated at NPL, UK and PTB, Germany. At both institutes an active hydrogen maser serves as a flywheel oscillator; it is connected to a GPS receiver as an external frequency reference and compared simultaneously to a realization of the unperturbed frequency of the ${{}^2S_{1/2}(F=0)-{}^2D_{3/2}(F=2)}$ electric quadrupole transition in ${}^{171}$Yb${}^+$ via an optical femtosecond frequency comb. To profit from long coherent GPS link measurements we extrapolate over the various data gaps in the optical clock to maser comparisons which introduces maser noise to the frequency comparison but improves the uncertainty from the GPS link. We determined the total statistical uncertainty consisting of the GPS link uncertainty and the extrapolation uncertainties for several extrapolation schemes. Using the extrapolation scheme with the smallest combined uncertainty, we find a fractional frequency difference $y(\mathrm{PTB})-y(\mathrm{NPL})$ of $-1.3(1.2)\times 10^{-15}$ for a total measurement time of 67 h. This result is consistent with an agreement of both optical clocks and with recent absolute frequency measurements against caesium fountain clocks., Comment: 5 pages, 3 figures

A method is presented for analysing over-determined sets of clock frequency comparison data involving standards based on a number of different reference transitions. This least-squares adjustment procedure, which is based on the method used by CODATA to derive a self-consistent set of values for the fundamental physical constants, can be used to derive optimized values for the frequency ratios of all possible pairs of reference transitions. It is demonstrated to reproduce the frequency values recommended by the International Committee for Weights and Measures, when using the same input data used to derive those values. The effects of including more recently published data in the evaluation is discussed and the importance of accounting for correlations between the input data is emphasised., Comment: 12 pages, 4 figures

Results are presented from a series of comparisons between two independent femtosecond frequency comb systems at NPL, which were carried out in order to assess their systematic uncertainty. Simultaneous measurements with the two systems demonstrate agreement at the level of 5 x $10^{-18}$ when measuring an optical frequency against a common microwave reference. When simultaneously measuring the ratio of two optical frequencies, agreement at the 3 x $10^{-21}$ level is observed. The results represent the highest reported level of agreement to date between Ti:sapphire and Er-doped femtosecond combs. The limitations of the combs when operating in these two different manners are discussed, including traceability to the SI second, which can be achieved with an uncertainty below 1 x $10^{-16}$. The technical details presented underpin recent absolute frequency measurements of the $^{88}$Sr$^+$ and $^{171}$Yb$^+$ optical clock transitions at NPL, as well as a frequency ratio measurement between the two optical clock transitions in $^{171}$Yb$^+$., Comment: 11 pages, 6 figures

Singly-ionized ytterbium, with ultra-narrow optical clock transitions at 467 nm and 436 nm, is a convenient system for the realization of optical atomic clocks and tests of present-day variation of fundamental constants. We present the first direct measurement of the frequency ratio of these two clock transitions, without reference to a cesium primary standard, and using the same single ion of 171Yb+. The absolute frequencies of both transitions are also presented, each with a relative standard uncertainty of $6\times 10^{-16}$. Combining our results with those from other experiments, we report a three-fold improvement in the constraint on the time-variation of the proton-to-electron mass ratio, $\dot{\mu}/{\mu} = 0.2(1.1)\times 10^{-16}$ year$^{-1}$, along with an improved constraint on time-variation of the fine structure constant, $\dot{\alpha}/{\alpha} = -0.7(2.1)\times 10^{-17}$ year$^{-1}$., Comment: 6 pages, 4 figures. Additional citations and minor changes after peer review

The performance of optical clocks has strongly progressed in recent years, and accuracies and instabilities of 1 part in 10^18 are expected in the near future. The operation of optical clocks in space provides new scientific and technological opportunities. In particular, an earth-orbiting satellite containing an ensemble of optical clocks would allow a precision measurement of the gravitational redshift, navigation with improved precision, mapping of the earth's gravitational potential by relativistic geodesy, and comparisons between ground clocks., Comment: Proc. III International Conference on Particle and Fundamental Physics in Space (SpacePart06), Beijing 19 - 21 April 2006, to appear in Nucl. Phys. B