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Multi-ion optical clocks offer the possibility of overcoming the low signal-to-noise ratio of single-ion clocks, while still providing low systematic uncertainties. We present simultaneous spectroscopy of up to four ${}^{115}$In${}^+$ clock ions in a linear Coulomb crystal, sympathetically cooled with ${}^{172}$Yb${}^+$ ions. In first clock comparisons, we see agreement below $1\times10^{-17}$ with results obtained using a single In${}^+$ ion, for which we have evaluated the systematic uncertainty to be $2.5\times10^{-18}$. Operation with four clock ions reduces the instability from $1.6\times10^{-15}/\sqrt{t/(1\;\mathrm{s})}$ to $9.2\times10^{-16}/\sqrt{t/(1\;\mathrm{s})}$. We derive a model for decay-related dead time during state preparation, which matches the observed scaling of instability with clock ion number $N$, and indicates that $1/\sqrt{N}$ scaling can be achieved with the addition of a repump laser., Comment: 7 pages, 4 figures

The 10-minute radiative lifetime of the first excited $^{229}$Th$^{4+}$ nuclear state in ionic crystals provides narrow spectroscopic linewidths, enabling the realization of a solid-state nuclear clock. Due to the 4+ noble gas configuration, electronic readout or state initialization schemes known from atomic clocks are inaccessible. This elongates the interrogation cycle, which will deteriorate the clock performance. To address this limitation we demonstrate laser-induced quenching (LIQ) as a method of depumping the $^{229}$Th isomer population in CaF$_2$. We provide experimental evidence for LIQ at different wavelengths (148 - 420 nm) and temperatures (100 - 350 K), achieving a threefold reduction in the isomer lifetime with 20 mW of laser power., Comment: 8 Pages, 8 Figures

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

Sympathetic cooling of Th$^{3+}$ ions is demonstrated in an experiment where $^{229}$Th and $^{230}$Th are extracted from uranium recoil ion sources and are confined in a linear Paul trap together with laser-cooled $^{88}$Sr$^+$ ions. Because of their similar charge-to-mass ratios the ions are closely coupled and arrange themselves in two-species Coulomb crystals, containing up to a few tens of Th$^{3+}$ ions. To show the suitability of the sympathetically cooled Th$^{3+}$ ions for high-resolution laser spectroscopy, the absolute frequencies and isotope shifts of 5F$_{5/2}$\,$\rightarrow$\,6D$_{5/2}$ and 5F$_{7/2}$\,$\rightarrow$\,6D$_{5/2}$ transitions of $^{230}$Th$^{3+}$ have been measured. The system is developed for hyperfine spectroscopy of electronic transitions of nuclear ground and isomeric states in $^{229}$Th$^{3+}$., Comment: 8 pages, 8 figures

The twisted light modes used in modern atomic physics experiments can be contaminated by small admixtures of plane wave radiation. Although these admixtures hardly reveal themselves in the beam intensity profile, they may seriously affect the outcome of high precision spectroscopy measurements. In the present study we propose a method for diagnosing such a plane wave contamination, which is based on the analysis of the magnetic sublevel population of atoms or ions interacting with the "twisted + plane wave" radiation. In order to theoretically investigate the sublevel populations, we solve the Liouville-von Neumann equation for the time evolution of atomic density matrix. The proposed method is illustrated for the electric dipole $5s \, {}^{2}\mathrm{S}_{1/2} \, - \, 5p \, {}^{2}\mathrm{P}_{3/2}$ transition in Rb induced by (linearly, radially, or azimuthally polarized) vortex light with just a small contamination. We find that even tiny admixtures of plane wave radiation can lead to remarkable variations in the populations of the ground-state magnetic sublevels. This opens up new opportunities for diagnostics of twisted light in atomic spectroscopy experiments., Comment: 12 pages, 11 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 present improved constraints on the coupling of ultralight bosonic dark matter to photons based on long-term measurements of two optical frequency ratios. In these optical clock comparisons, we relate the frequency of the ${}^2S_{1/2} (F=0)\leftrightarrow {}^2F_{7/2} (F=3)$ electric-octupole (E3) transition in $^{171}$Yb$^{+}$ to that of the ${}^2S_{1/2} (F=0)\leftrightarrow \,{}^2D_{3/2} (F=2)$ electric-quadrupole (E2) transition of the same ion, and to that of the ${}^1S_0\leftrightarrow\,{}^3P_0$ transition in $^{87}$Sr. Measurements of the first frequency ratio $\nu_\textrm{E3}/\nu_\textrm{E2}$ are performed via interleaved interrogation of both transitions in a single ion. The comparison of the single-ion clock based on the E3 transition with a strontium optical lattice clock yields the second frequency ratio $\nu_\textrm{E3}/\nu_\textrm{Sr}$. By constraining oscillations of the fine-structure constant $\alpha$ with these measurement results, we improve existing bounds on the scalar coupling $d_e$ of ultralight dark matter to photons for dark matter masses in the range of about $ 10^{-24}-10^{-17}\,\textrm{eV}/c^2$. These results constitute an improvement by more than an order of magnitude over previous investigations for most of this range. We also use the repeated measurements of $\nu_\textrm{E3}/\nu_\textrm{E2}$ to improve existing limits on a linear temporal drift of $\alpha$ and its coupling to gravity., Comment: 7 pages, 5 figures

We report on an evaluation of an optical clock that uses the $\phantom{}^2S_{1/2} \rightarrow \phantom{}^2D_{5/2}$ transition of a single $^{88}$Sr$^+$ ion as the reference. In contrast to previous work, we estimate the effective temperature of the blackbody radiation that shifts the reference transition directly during operation from the corresponding frequency shift and the well-characterized sensitivity to thermal radiation. We measure the clock output frequency against an independent $^{171}$Yb$^+$ ion clock, based on the $\phantom{}^2S_{1/2} (F=0) \rightarrow \phantom{}^2F_{7/2} (F=3)$ electric octupole (E3) transition, and determine the frequency ratio with a total fractional uncertainty of $2.3\times 10^{-17}$. Relying on a previous measurement of the $^{171}$Yb$^+$ (E3) clock frequency, we find the absolute frequency of the $^{88}$Sr$^+$ clock transition to be $444779044095485.271(59)\,\text{Hz}$. Our result reduces the uncertainty by a factor of $3$ compared to the previously most accurate measurement and may help to resolve so far inconsistent determinations of this value. We also show that for three simultaneously interrogated $^{88}$Sr$^+$ ions, the increased number causes the expected improvement of the short-term frequency instability of the optical clock without degrading its systematic uncertainty., Comment: 6 pages, 4 figures

The last decade has seen unprecedented effort in dark matter model building at all mass scales coupled with the design of numerous new detection strategies. Transformative advances in quantum technologies have led to a plethora of new high-precision quantum sensors and dark matter detection strategies for ultralight ($<10\,$eV) bosonic dark matter that can be described by an oscillating classical, largely coherent field. This white paper focuses on searches for wavelike scalar and vector dark matter candidates., Comment: Snowmass 2021 White Paper

We report a measurement of the radiative lifetime of the $^2F_{7/2}$ level of $^{171}$Yb$^+$ that is coupled to the $^2S_{1/2}$ ground state via an electric octupole transition. The radiative lifetime is determined to be $4.98(25)\times 10^7$ s, corresponding to 1.58(8) years. The result reduces the relative uncertainty in this exceptionally long excited state lifetime by one order of magnitude with respect to previous experimental estimates. Our method is based on the coherent excitation of the corresponding transition and avoids limitations through competing decay processes. The explicit dependence on the laser intensity is eliminated by simultaneously measuring the resonant Rabi frequency and the induced quadratic Stark shift. Combining the result with information on the dynamic differential polarizability permits a calculation of the transition matrix element to infer the radiative lifetime., Comment: 5 pages, 2 figures

The low-energy, long-lived isomer in $^{229}$Th, first studied in the 1970s as an exotic feature in nuclear physics, continues to inspire a multidisciplinary community of physicists. Using the nuclear resonance frequency, determined by the strong and electromagnetic interactions inside the nucleus, it is possible to build a highly precise nuclear clock that will be fundamentally different from all other atomic clocks based on resonant frequencies of the electron shell. The nuclear clock will open opportunities for highly sensitive tests of fundamental principles of physics, particularly in searches for violations of Einstein's equivalence principle and for new particles and interactions beyond the standard model. It has been proposed to use the nuclear clock to search for variations of the electromagnetic and strong coupling constants and for dark matter searches. The $^{229}$Th nuclear optical clock still represents a major challenge in view of the tremendous gap of nearly 17 orders of magnitude between the present uncertainty in the nuclear transition frequency and the natural linewidth. Significant experimental progress has been achieved in recent years, which will be briefly reviewed. Moreover, a research strategy will be outlined to consolidate our present knowledge about essential $^{229\rm{m}}$Th properties, to determine the nuclear transition frequency with laser spectroscopic precision, realize different types of nuclear clocks and apply them in precision frequency comparisons with optical atomic clocks to test fundamental physics. Two avenues will be discussed: laser-cooled trapped $^{229}$Th ions that allow experiments with complete control on the nucleus-electron interaction and minimal systematic frequency shifts, and Th-doped solids enabling experiments at high particle number and in different electronic environments., Comment: 34 pages

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 introduce a scheme to coherently suppress second-rank tensor frequency shifts in atomic clocks, relying on the continuous rotation of an external magnetic field during the free atomic state evolution in a Ramsey sequence. The method retrieves the unperturbed frequency within a single interrogation cycle and is readily applicable to various atomic clock systems. For the frequency shift due to the electric quadrupole interaction, we experimentally demonstrate suppression by more than two orders of magnitude for the ${}^2S_{1/2} \to {}^2D_{3/2}$ transition of a single trapped ${}^{171}\text{Yb}^+$ ion. The scheme provides particular advantages in the case of the ${}^{171}\text{Yb}^+$ ${}^2S_{1/2} \to {}^2F_{7/2}$ electric octupole (E3) transition. For an improved estimate of the residual quadrupole shift for this transition, we measure the excited state electric quadrupole moments $\Theta({}^2D_{3/2}) = 1.95(1)~ea_0^2$ and $\Theta({}^2F_{7/2}) = -0.0297(5)~ea_0^2$ with $e$ the elementary charge and $a_0$ the Bohr radius, improving the measurement uncertainties by one order of magnitude., Comment: 6 pages, 3 figures

A theoretical study is performed for the excitation of a single atom localized in the center of twisted light modes. Here we present the explicit dependence of excitation rates on critical parameters, such as the polarization of light, its orbital angular momentum projection, and the orientation of its propagation axis with respect to the atomic quantization axis. The effect of a spatial spread of the atom is also considered in detail. The expressions for transition rates obtained in this work can be used for any atom of arbitrary electronic configuration. For definiteness we apply them to the specific case of $^{2}S_{1/2} (F=0) \rightarrow\; ^{2}F_{7/2} (F=3, M=0)$ electric octupole (E3) transition in $^{171}$Yb$^{+}$ ion. Our analytical and numerical results are suitable for the analysis and planning of future experiments on the excitation of electric-dipole-forbidden transitions by twisted light modes in optical atomic clocks.

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.

The isotope $^{229}$Th is unique in that it possesses an isomeric state of only a few eV above the ground state, suitable for nuclear laser excitation. An optical clock based on this transition is expected to be a very sensitive probe for variations of fundamental constants, but the nuclear properties of both states have to be determined precisely to derive the actual sensitivity. We carry out isotope shift calculations in Th$^+$ and Th$^{2+}$ including the specific mass shift, using a combination of configuration interaction and all-order linearized coupled-cluster methods and estimate the uncertainty of this approach. We perform experimental measurements of the hyperfine structure of Th$^{2+}$ and isotopic shift between $^{229}$Th$^{2+}$ and $^{232}$Th$^{2+}$ to extract the difference in root-mean-square radii as $\delta \langle r^{2} \rangle^{232,229}=0.299(15)$ fm$^2$. Using the recently measured values of the isomer shift of lines of $^{229\textrm{m}}$Th, we derive the value for the mean-square radius change between $^{229}$Th and its low lying isomer $^{229\textrm{m}}$Th to be $\delta \langle r^2 \rangle^{229\textrm{m},229} = 0.0105(13)\,{\rm fm}^2$., Comment: 5 pages, 2 figures

We experimentally investigate an optical frequency standard based on the $^2S_{1/2} (F=0)\to {}^2F_{7/2} (F=3)$ electric octupole (\textit{E}3) transition of a single trapped $^{171}$Yb$^+$ ion. For the spectroscopy of this strongly forbidden transition, we utilize a Ramsey-type excitation scheme that provides immunity to probe-induced frequency shifts. The cancellation of these shifts is controlled by interleaved single-pulse Rabi spectroscopy which reduces the related relative frequency uncertainty to $1.1\times 10^{-18}$. To determine the frequency shift due to thermal radiation emitted by the ion's environment, we measure the static scalar differential polarizability of the \textit{E}3 transition as $0.888(16)\times 10^{-40}$ J m$^2$/V$^2$ and a dynamic correction $\eta(300~\text{K})=-0.0015(7)$. This reduces the uncertainty due to thermal radiation to $1.8\times 10^{-18}$. The residual motion of the ion yields the largest contribution $(2.1\times 10^{-18})$ to the total systematic relative uncertainty of the clock of $3.2\times 10^{-18}$., Comment: 5 pages, 4 figures

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

We have measured the hyperfine structure and isotope shifts of the 402.0 nm and 399.6 nm resonance lines in 229Th+. These transitions could provide pathways towards the 229Th isomeric nuclear state excitation. An unexpected negative isotope shift relative to 232Th+ is observed for the 399.6 nm line, indicating a strong Coulomb coupling of the excited state to the nucleus. We have developed a new all-order approach to the isotope shift calculations that is generally applicable to heavy atoms and ions with several valence electrons. The theoretical calculations provide an explanation for the negative isotope shift of the 399.6 nm transition and yield a corrected classification of the excited state. The calculated isotope shifts are in good agreement with experimental values., Comment: 5 pages, 2 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

Using resonant two-step laser excitation of trapped 232Th+ ions, we observe 43 previously unknown energy levels within the energy range from 7.3 to 8.3 eV. The high density of states promises a strongly enhanced electronic bridge excitation of the 229mTh nuclear state that is expected in this energy range. From the observation of resonantly enhanced three-photon ionization of Th+, the second ionization potential of thorium can be inferred to lie within the range between 11.9 and 12.3 eV. Pulsed laser radiation in a wide wavelength range from 237 to 289 nm is found to provide efficient photodissociation of molecular ions that are formed in reactions of Th+ with impurities in the buffer gas, leading to a significantly increased storage time for Th+ in the ion trap., Comment: 7 pages, 6 figures

We experimentally investigate a recently proposed optical excitation scheme [V.I. Yudin et al., Phys. Rev. A 82, 011804(R)(2010)] that is a generalization of Ramsey's method of separated oscillatory fields and consists of a sequence of three excitation pulses. The pulse sequence is tailored to produce a resonance signal which is immune to the light shift and other shifts of the transition frequency that are correlated with the interaction with the probe field. We investigate the scheme using a single trapped 171Yb+ ion and excite the highly forbidden 2S1/2-2F7/2 electric-octupole transition under conditions where the light shift is much larger than the excitation linewidth, which is in the Hertz range. The experiments demonstrate a suppression of the light shift by four orders of magnitude and an immunity against its fluctuations., Comment: 5 pages, 4 figures

Experiments on one- and two-photon laser excitation of 232Th+ ions in a radiofrequency ion trap are reported. As the first excitation step, the strongest resonance line at 402 nm from the 6d^2 7s J=3/2 ground state to the 6d7s7p J=5/2 state at 24874 cm^{-1} is driven by radiation from an extended cavity diode laser. Spontaneous decay of the intermediate state populates a number of low-lying metastable states, thus limiting the excited state population and fluorescence signal obtainable with continuous laser excitation. We study the collisional quenching efficiency of helium, argon, and nitrogen buffer gases, and the effect of repumping laser excitation from the three lowest-lying metastable levels. The experimental results are compared with a four-level rate equation model, that allows us to deduce quenching rates for these buffer gases. Using laser radiation at 399 nm for the second step, we demonstrate two-photon excitation to the state at 49960 cm^{-1}, among the highest-lying classified levels of Th+. This is of interest as a test case for the search for higher-lying levels in the range above 55000 cm^{-1} which can resonantly enhance the excitation of the 229Th+ nuclear resonance through an inverse two-photon electronic bridge process., Comment: 8 pages, 8 figures

The production of ions via laser ablation for the loading of radiofrequency (RF) ion traps is investigated using a nitrogen laser with a maximum pulse energy of 0.17 mJ and a peak intensity of about 250 MW/cm^2. A time-of-flight mass spectrometer is used to measure the ion yield and the distribution of the charge states. Singly charged ions of elements that are presently considered for the use in optical clocks or quantum logic applications could be produced from metallic samples at a rate of the order of magnitude 10^5 ions per pulse. A linear Paul trap was loaded with Th+ ions produced by laser ablation. An overall ion production and trapping efficiency of 10^-7 to 10^-6 was attained. For ions injected individually, a dependence of the capture probability on the phase of the RF field has been predicted. In the experiment this was not observed, presumably because of collective effects within the ablation plume., Comment: submitted to Appl. Phys. B., special issue on ion trapping

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 develop a nonstandard concept of atomic clocks where the blackbody radiation shift (BBRS) and its temperature fluctuations can be dramatically suppressed (by one to three orders of magnitude) independent of the environmental temperature. The suppression is based on the fact that in a system with two accessible clock transitions (with frequencies v1 and v2) which are exposed to the same thermal environment, there exists a "synthetic" frequency v_{syn} (v1-e12 v2) largely immune to the BBRS. As an example, it is shown that in the case of ion 171Yb+ it is possible to create a clock in which the BBRS can be suppressed to the fractional level of 10^{-18} in a broad interval near room temperature (300\pm 15 K). We also propose a realization of our method with the use of an optical frequency comb generator stabilized to both frequencies v1 and v2. Here the frequency v_{syn} is generated as one of the components of the comb spectrum and can be used as an atomic standard., Comment: 5 pages, 2 figures

We consider the excitation of the nuclear transition ^{229g}Th - ^{229m}Th near 7.6 eV in singly ionized thorium via an electronic bridge process. The process relies on the excitation of the electron shell by two laser photons whose sum frequency is equal to the nuclear transition frequency. This scheme allows to determine the nuclear transition frequency with high accuracy. Based on calculations of the electronic level structure of Th^+ which combine the configuration-interaction method and many-body perturbation theory, we estimate that a nuclear excitation rate in the range of 10 s^{-1} can be obtained using conventional laser sources., Comment: 4 pages, 3 figures

The 7.6-eV-isomer of Thorium-229 offers the opportunity to perform high resolution laser spectroscopy of a nuclear transition. We give a brief review of the investigations of this isomer. The nuclear resonance connecting ground state and isomer may be used as the reference of an optical clock of very high accuracy using trapped and laser-cooled thorium ions, or in a compact solid-state optical frequency standard of high stability., Comment: 5 pages, 1 figure; Proceedings of the 7th Symposium on Frequency Standards and Metrology, 5-11 October 2008; reference added for section 3

We summarise the scientific and technological aspects of the SAGAS (Search for Anomalous Gravitation using Atomic Sensors) project, submitted to ESA in June 2007 in response to the Cosmic Vision 2015-2025 call for proposals. The proposed mission aims at flying highly sensitive atomic sensors (optical clock, cold atom accelerometer, optical link) on a Solar System escape trajectory in the 2020 to 2030 time-frame. SAGAS has numerous science objectives in fundamental physics and Solar System science, for example numerous tests of general relativity and the exploration of the Kuiper belt. The combination of highly sensitive atomic sensors and of the laser link well adapted for large distances will allow measurements with unprecedented accuracy and on scales never reached before. We present the proposed mission in some detail, with particular emphasis on the science goals and associated measurements., Comment: 39 pages. Submitted in abridged version to Experimental Astronomy

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

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

We describe experiments with an optical frequency standard based on a laser cooled $^{171}$Yb$^+$ ion confined in a radiofrequency Paul trap. The electric-quadrupole transition from the $^2S_{1/2}(F=0)$ ground state to the $^2D_{3/2}(F=2)$ state at the wavelength of 436 nm is used as the reference transition. In order to compare two $^{171}$Yb$^+$ standards, separate frequency servo systems are employed to stabilize two probe laser frequencies to the reference transition line centers of two independently stored ions. The experimental results indicate a relative instability (Allan standard deviation) of the optical frequency difference between the two systems of $\sigma_y(1000 {\rm s})=5\cdot 10^{-16}$ only, so that shifts in the sub-hertz range can be resolved. Shifts of several hertz are observed if a stationary electric field gradient is superimposed on the radiofrequency trap field. The absolute optical transition frequency of Yb$^+$ at 688 THz was measured with a cesium atomic clock at two times separated by 2.8 years. A temporal variation of this frequency can be excluded within a $1\sigma$ relative uncertainty of $4.4\cdot 10^{-15}$ yr$^{-1}$. Combined with recently published values for the constancy of other transition frequencies this measurement provides a limit on the present variability of the fine structure constant $\alpha$ at the level of $2.0\cdot 10^{-15}$ yr$^{-1}$., Comment: 12 pages, 5 figures, Proceedings of MPLP'04, Novosibirsk, August 22.-27., 2004

The comparison of different atomic transition frequencies over time can be used to determine the present value of the temporal derivative of the fine structure constant alpha in a model-independent way without assumptions on constancy or variability of other parameters. We have measured an optical transition frequency at 688 THz in ^{171}Yb+ with a cesium atomic clock at two times separated by 2.8 years and find a value for the fractional variation of the frequency ratio $f_{\rm Yb}/f_{\rm Cs}$ of $(-1.2\pm 4.4)\cdot 10^{-15}$ yr$^{-1}$, consistent with zero. Combined with recently published values for the constancy of other transition frequencies this measurement sets an upper limit on the present variability of alpha at the level of $2.0\cdot 10^{-15}$ yr$^{-1}$, corresponding so far to the most stringent limit from laboratory experiments., Comment: 4 pages, 3 figures, references updated

We describe experimental investigations on an optical frequency standard based on a laser cooled 171Yb+ ion confined in a radiofrequency Paul trap. The electric-quadrupole transition from the 2S1/2(F=0) ground state to the 2D3/2(F=2) state at the wavelength of 436 nm is used as the reference transition. The reference transition is probed by a frequency-doubled, frequency-stabilized diode laser and is resolved with a Fourier-limited full halfwidth of approximately 30 Hz. In order to compare two 171Yb+ standards, separate frequency shift and servo systems are employed to stabilise the probe frequency to the reference transition line centers of two independently stored 171Yb+ ions. The present experimental results indicate a relative instability (Allan standard deviation)of the optical frequency difference between the two systems of sigma_y(1000 s)=1.0E-15 and a mean frequency difference of 0.2 Hz. Shifts in the range of several Hertz are observed in the frequency difference if a stationary electric field gradient is superimposed on the radiofrequency trap field. This measurement permits a first experimental estimate of the electric quadrupole moment of the 2D3/2 state of Yb+., Comment: To appear in "Laser Spectroscopy XVI", eds: P. Hannaford, A. Sidorov, H. Bachor, and K. Baldwin (World Scientific, Singapore, 2004)

The absolute frequency of the In$^{+}$ $5s^{2 1}S_{0}$ - $5s5p^{3}P_{0}$ clock transition at 237 nm was measured with an accuracy of 1.8 parts in $10^{13}$. Using a phase-coherent frequency chain, we compared the $^{1}S_{0}$ - $^{3}P_{0}$ transition with a methane-stabilized He-Ne laser at 3.39 $\mu$m which was calibrated against an atomic cesium fountain clock. A frequency gap of 37 THz at the fourth harmonic of the He-Ne standard was bridged by a frequency comb generated by a mode-locked femtosecond laser. The frequency of the In$^{+}$ clock transition was found to be $1 267 402 452 899.92 (0.23)$ kHz, the accuracy being limited by the uncertainty of the He-Ne laser reference. This represents an improvement in accuracy of more than 2 orders of magnitude on previous measurements of the line and now stands as the most accurate measurement of an optical transition in a single ion., Comment: 3 pages, 2 figures. accepted for publication in Opt. Lett