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We present a scalable mixed-species Coulomb crystal clock based on the $^1S_0$ $\leftrightarrow$ $^3P_0$ transition in $^{115}$In$^+$. $^{172}$Yb$^+$ ions are co-trapped and used for sympathetic cooling. Reproducible interrogation conditions for mixed-species Coulomb crystals are ensured by a conditional preparation sequence with permutation control. We demonstrate clock operation with a 1In$^+$-3Yb$^+$ crystal, achieving a relative systematic uncertainty of $2.5\times10^{-18}$ and a relative frequency instability of $1.6\times10^{-15}/\sqrt{\tau/1\;\mathrm{s}}$. We report on absolute frequency measurements with an uncertainty of $1.3\times10^{-16}$ and optical frequency comparisons with clocks based on $^{171}$Yb$^+$ (E3) and $^{87}$Sr. With a fractional uncertainty of $4.4\times10^{-18}$, the former is - to our knowledge - the most accurate frequency ratio value reported to date. For the $^{115}$In$^+$/$^{87}$Sr ratio, we improve upon the best previous measurement by more than an order of magnitude. We also demonstrate operation with four $^{115}$In$^+$ clock ions, which reduces the instability to $9.2\times10^{-16}/\sqrt{\tau/1\;\mathrm{s}}$., Comment: 13 pages, 10 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

We compare two optical clocks based on the $^2$S$_{1/2}(F=0)\to {}^2$D$_{3/2}(F=2)$ electric quadrupole (E2) and the $^2$S$_{1/2}(F=0)\to {}^2$F$_{7/2}(F=3)$ electric octupole (E3) transition of $^{171}$Yb$^{+}$ and measure the frequency ratio $\nu_{\mathrm{E3}}/\nu_{\mathrm{E2}}=0.932\,829\,404\,530\,965\,376(32)$. We determine the transition frequency $\nu_{E3}=642\,121\,496\,772\,645.10(8)$ Hz using two caesium fountain clocks. Repeated measurements of both quantities over several years are analyzed for potential violations of local position invariance. We improve by factors of about 20 and 2 the limits for fractional temporal variations of the fine structure constant $\alpha$ to $1.0(1.1)\times10^{-18}/\mathrm{yr}$ and of the proton-to-electron mass ratio $\mu$ to $-8(36)\times10^{-18}/\mathrm{yr}$. Using the annual variation of the Sun's gravitational potential at Earth $\Phi$, we improve limits for a potential coupling of both constants to gravity, $(c^2/\alpha) (d\alpha/d\Phi)=14(11)\times 10^{-9}$ and $(c^2/\mu) (d\mu/d\Phi)=7(45)\times 10^{-8}$., Comment: 6 pages, 3 figures

We report on a series of 42 measurements of the transition frequency of the 429~THz (5s$^2$)~$^1$S$_0$--(5s5p)~$^3$P$_0$ line in $^{87}$Sr taken over three years from 2017 to 2019. They have been performed at the Physikalisch-Technische Bundesanstalt (PTB) between the laboratory strontium lattice clock and the primary caesium fountain clocks CSF1 and CSF2. The length of each individual measurement run has been extended by use of a hydrogen maser as flywheel to improve the statistical uncertainty given by the Cs clocks. We determine an averaged transition frequency of $429\:228\:004\:229\:873.00(0.07)$~Hz with $1.5\times10^{-16}$ fractional uncertainty, at the limit of the current realization of the unit hertz. Analysis of the data provides an improved limit on the coupling of the gravitational potential of the Sun to the proton--electron mass ratio $\mu$, and confirms the limits on its temporal drift., Comment: 8 pages, 4 figures

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

Improvements of the systematic uncertainty, frequency instability, and long-term reliability of the two caesium fountain primary frequency standards CSF1 and CSF2 at PTB (Physikalisch-Technische Bundesanstalt) are described. We have further investigated many of the systematic effects and made a number of modifications of the fountains. With an optically stabilized microwave oscillator, the quantum projection noise limited frequency instabilities are improved to $7.2 \times 10^{-14} (\tau/1\,\mathrm{s})^{-1/2}$ for CSF1 and $2.5 \times 10^{-14} (\tau/1\,\mathrm{s})^{-1/2}$ for CSF2 at high atom density. The systematic uncertainties of CSF1 and CSF2 are reduced to $2.74 \times 10^{-16}$ and $1.71 \times 10^{-16}$, respectively. Both fountain clocks regularly calibrate the scale unit of International Atomic Time (TAI) and the local realization of Coordinated Universal Time, UTC(PTB), and serve as references to measure the frequencies of local and remote optical frequency standards., Comment: 33 pages, 7 figures

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.

Optical clocks are not only powerful tools for prime fundamental research, but are also deemed for the re-definition of the SI base unit second as they now surpass the performance of caesium atomic clocks in both accuracy and stability by more than an order of magnitude. However, an important obstacle in this transition has so far been the limited reliability of the optical clocks that made a continuous realization of a timescale impractical. In this paper, we demonstrate how this situation can be resolved and that a timescale based on an optical clock can be established that is superior to one based on even the best caesium fountain clocks. The paper also gives further proof of the international consistency of strontium lattice clocks on the $10^{-16}$ accuracy level, which is another prerequisite for a change in the definition of the second.

Coherent manipulation of atomic states is a key concept in high-precision spectroscopy and used in atomic fountain clocks and a number of optical frequency standards. Operation of these standards can involve a number of cyclic switching processes, which may induce cycle synchronous phase excursions of the interrogation signal and thus lead to shifts in the output of the frequency standard. We have built a FPGA-based phase analyzer to investigate these effects and conducted measurements on two frequency standards. For the caesium fountain PTB-CSF2 we were able to exclude phase variations of the microwave source at the level of a few $\mu$rad, corresponding to relative frequency shifts of less than 10$^{-16}$. In the optical domain, we investigated phase variations in PTB's Yb$^+$ optical frequency standard and made detailed measurements of AOM chirps and their scaling with duty cycle and driving power. We ascertained that cycle-synchronous as well as long-term phase excursion do not cause frequency shifts larger than 10$^{-18}$., Comment: 5 pages, 4 figures

Accurate measurements of different transition frequencies between atomic levels of the electronic and hyperfine structure over time are used to investigate temporal variations of the fine structure constant $\alpha$ and the proton-to-electron mass ratio $\mu$. We measure the frequency of the $^2S_{1/2}\rightarrow {^2F_{7/2}}$ electric octupole (E3) transition in $^{171}$Yb$^+$ against two caesium fountain clocks as $f(E3) = 642\,121\,496\,772\,645.36(25)$~Hz with an improved fractional uncertainty of $3.9\times 10^{-16}$. This transition frequency shows a strong sensitivity to changes of $\alpha$. Together with a number of previous and recent measurements of the $^2S_{1/2}\rightarrow {^2D_{3/2}}$ electric quadrupole transition in $^{171}$Yb$^+$ and with data from other elements, a least-squares analysis yields $(1/\alpha)(d\alpha/dt)=-0.20(20)\times 10^{-16}/\mathrm{yr}$ and $(1/\mu)(d\mu/dt)=-0.5(1.6)\times 10^{-16}/\mathrm{yr}$, confirming a previous limit on $d\alpha/dt$ and providing the most stringent limit on $d \mu/dt$ from laboratory experiments., Comment: 5 pages, 3 figures

We describe a measurement of the frequency of the 2S1/2(F = 0) - 2D3/2(F' = 2) transition of 171Yb+ at the wavelength 436 nm (frequency 688 THz), using a single Yb+ ion confined in a Paul trap and two caesium fountains as references. In one of the fountains, the frequency of the microwave oscillator that interrogates the caesium atoms is stabilized by the laser that excites the Yb+ reference transition with a linewidth in the hertz range. The stability is transferred to the microwave oscillator with the use of a fiber laser based optical frequency comb generator that also provides the frequency conversion for the absolute frequency measurement. The frequency comb generator is configured as a transfer oscillator so that fluctuations of the pulse repetition rate and of the carrier offset frequency do not degrade the stability of the frequency conversion. The phase noise level of the generated ultrastable microwave signal is comparable to that of a cryogenic sapphire oscillator. For fountain operation with optical molasses loaded from a laser cooled atomic beam source, we obtain a stability corresponding to a fractional Allan deviation of $4.1\times 10^{-14}\ (\tau/\text{s})^{-1/2}$. With the molasses loaded from thermal vapor and an averaging time of 65 h, we measure the frequency of the Yb+ transition with a relative statistical uncertainty of $2.8\times10^{-16}$ and a systematic uncertainty of $5.9\times10^{-16}$. The frequency was also simultaneously measured with the second fountain that uses a quartz-based interrogation oscillator. The unperturbed frequency of the Yb+ transition is realized with an uncertainty of $1.1\times10^{-16}$ that mainly results from the uncertainty of the blackbody shift at the operating temperature near 300 K. The transition frequency of 688 358 979 309 307.82(36) Hz, measured with the two fountains, is in good agreement with previous results., Comment: 25 pages, 4 figures. Submitted to Phys. Rev. A

We experimentally investigate an optical frequency standard based on the 467 nm (642 THz) electric-octupole reference transition 2S1/2(F=0) -> F7/2(F=3) in a single trapped 171Yb+ ion. The extraordinary features of this transition result from the long natural lifetime and from the 4f136s2 configuration of the upper state. The electric quadrupole moment of the 2F7/2 state is measured as -0.041(5) e(a0)^2, where e is the elementary charge and a0 the Bohr radius. We also obtain information on the differential scalar and tensorial components of the static polarizability and of the probe light induced ac Stark shift of the octupole transition. With a real-time extrapolation scheme that eliminates this shift, the unperturbed transition frequency is realized with a fractional uncertainty of 7.1x10^(-17). The frequency is measured as 642 121 496 772 645.15(52) Hz., Comment: 5 pages, 4 figures

We evaluate the frequency error from distributed cavity phase in the caesium fountain clock PTB-CSF2 at the Physikalisch-Technische Bundesanstalt with a combination of frequency measurements and ab initio calculations. The associated uncertainty is 1.3E-16, with a frequency bias of 0.4E-16. The agreement between the measurements and calculations explains the previously observed frequency shifts at elevated microwave amplitude. We also evaluate the frequency bias and uncertainty due to the microwave lensing of the atomic wavepackets. We report a total PTB-CSF2 systematic uncertainty of 4.1E-16., Comment: 15 pages, 5 figures, to be published in Metrologia

We perform Ramsey-Bord\'e spectroscopy on laser-cooled magnesium atoms in free fall to measure the 1S0 \rightarrow 3P1 intercombination transition frequency. The measured value of 655 659 923 839 730 (48) Hz is consistent with our former atomic beam measurement (Friebe et al 2008 Phys. Rev. A 78 033830). We improve upon the fractional accuracy of the previous measurement by more than an order of magnitude to 7e-14. The magnesium frequency standard was referenced to a fountain clock of the Physikalisch-Technische Bundesanstalt (PTB) via a phase-stabilized telecom fiber link and its stability was characterized for interrogation times up to 8000 s. The high temperature of the atomic ensemble leads to a systematic shift due to the motion of atoms across the spectroscopy beams. In our regime, this leads to a counterintuitive reduction of residual Doppler shift with increasing resolution. Our theoretical model of the atom-light interaction is in agreement with the observed effect and allows us to quantify its contribution in the uncertainty budget., Comment: 16 pages, 8 figures. Accepted in New Journal of Physics

With 87-Sr atoms confined in a one dimensional optical lattice, the frequency of the optical clock transition 5s^2 ^1S_0 - 5s5p ^3P_0 has been determined to be 429 228 004 229 872.9(5) Hz. The transition frequency was measured with the help of a fs-frequency comb against one of PTB's H-masers whose frequency was measured simultaneously by the PTB Cs fountain clock CSF1. The Sr optical frequency standard contributes with a fractional uncertainty of 1.5 10^-16 to the total uncertainty. The agreement of the measured transition frequency with previous measurements at other institutes supports the status of this transition as secondary representation of the second with the currently smallest uncertainty., Comment: 9 pages, 6 figures

A caesium fountain clock is operated utilizing a microwave oscillator that derives its frequency stability from a stable laser by means of a fiber-laser femtosecond frequency comb. This oscillator is based on the technology developed for optical clocks and replaces the quartz based microwave oscillator commonly used in fountain clocks. As a result, a significant decrease of the frequency instability of the fountain clock is obtained, reaching 0.74E-14 at 100 s averaging time. We could demonstrate that for a significant range of detected atom numbers the instability is limited by quantum projection noise only, and that for the current status of this fountain clock the new microwave source poses no limit on the achievable frequency instability., Comment: 4 pages, 4 figures

We stabilise a microwave oscillator at 9.6 GHz to an optical clock laser at 344 THz by using a fibre-based femtosecond laser frequency comb as a transfer oscillator. With a second frequency comb we measure independently the instability of the microwave source with respect to another optical clock laser frequency at 456 THz. The total fractional frequency instability of this optic-to-microwave and microwave-to-optic conversion resulted in an Allan deviation sigma_y, of sigma_y=1.2E-14 at 1 s averaging time (band width 50 kHz). The residual phase noise density is -97 dBc/Hz at 10 Hz offset from the 9.6 GHz carrier. Replacing the existing quartz-based interrogation oscillator of the PTB caesium fountain CSF1 with this optically stabilised microwave source will reduce the instability contribution due to the Dick effect from the 1E-13-level at 1s averaging time to an insignificant level at the current status of CSF1. Therefore this new microwave source can be an alternative to cryogenic sapphire-loaded cavity oscillators in order to overcome the limitations of state-of-the-art quartz oscillators.

We have observed that the collisional frequency shift in primary caesium fountain clocks varies with the clock state population composition and, in particular, is zero for a given fraction of the |F = 4, mF = 0> atoms, depending on the initial cloud parameters. We present a theoretical model explaining our observations. The possibility of the collisional shift cancellation implies an improvement in the performance of caesium fountain standards and a simplification in their operation. Our results also have implications for test operation of fountains at multiple pi/2 pulse areas.

Precision comparisons of different atomic frequency standards over a period of a few years can be used for a sensitive search for temporal variations of fundamental constants. We present recent frequency measurements of the 688 THz transition in the $^{171}$Yb$^+$ ion. For this transition frequency a record over six years is now available, showing that a possible frequency drift relative to a cesium clock can be constrained to $(-0.54\pm0.97)$ Hz/yr, i.e. at the level of $2\cdot10^{-15}$ per year. Combined with precision frequency measurements of an optical frequency in $^{199}$Hg$^+$ and of the hyperfine ground state splitting in $^{87}$Rb a stringent limit on temporal variations of the fine structure constant $\alpha$: $d\ln\alpha /dt= (-0.26\pm0.39)\cdot 10^{-15} {\rm yr}^{-1}$ and a model-dependent limit for variations of the proton-to-electron mass ratio $\mu$ in the present epoch can be derived: $d \ln \mu/dt = (-1.2 \pm 2.2)\cdot 10^{-15} {\rm yr}^{-1}$. We discuss these results in the context of astrophysical observations that apparently indicate changes in both of these constants over the last 5--10 billion years., Comment: 10 pages, 3 figures, Proceedings of the 11th Marcel Grossmann Meeting, Berlin, 2006