Recent experimental progress in cooling, trapping, and quantum logic spectroscopy of highly-charged ions (HCIs) made HCIs accessible for high resolution spectroscopy and precision fundamental studies. Based on these achievements, we explore a possibility to develop optical clocks using transitions between the ground and a low-lying excited state in the Cf$^{15+}$ and Cf$^{17+}$ ions. Using a high-accuracy relativistic method of calculation we predicted the wavelengths of clock transitions, calculated relevant atomic properties, and analyzed a number of systematic effects (such as the electric quadrupole-, micromotion-, and quadratic Zeeman shifts of the clock transitions) that affect the accuracy and stability of the optical clocks. We also calculated magnetic dipole hyperfine-structure constants of the clock states and the blackbody radiation shifts of the clock transitions.
Al$^+$ ions optical clock is a very promising optical frequency standard candidate due to its extremely small blackbody radiation shift. It has been successfully demonstrated with indirect cooled, quantum-logic-based spectroscopy technique. Its accuracy is limited by second-order Doppler shift, and its stability is limited by the number of ions that can be probed in quantum logic processing. We propose a direct laser cooling scheme of Al$^+$ ions optical clocks where both the stability and accuracy of the clocks are greatly improved. In the proposed scheme, two Al$^+$ ions traps are utilized. …
We review a number of highly charged ions which have optical transitions suitable for building extremely accurate atomic clocks. This includes ions from Hf$^{12+}$ to U$^{34+}$, which have the $4f^{12}$ configuration of valence electrons, the Ir$^{17+}$ ion, which has a hole in almost filled $4f$ subshell, the Ho$^{14+}$, Cf$^{15+}$, Es$^{17+}$ and Es$^{16+}$ ions. Clock transitions in most of these ions are sensitive to variation of the fine structure constant, $α$ ($α= e^2/\hbar c$). E.g., californium and einsteinium ions have largest known sensitivity to $α$-variation while holmium ion look…
We identify laser-accessible transitions in group 16-like highly charged ions as candidates for high-accuracy optical clocks, including S-, Se-, and Te-like systems. For this class of ions, the ground $^{3}P_{J}$ fine structure manifold exhibits irregular (nonmonotonic in $J$) energy ordering for large enough ionization degree. We consider the $|^3P_2\rangle \longleftrightarrow |^3P_0\rangle$ (ground to first-excited state) electric quadrupole transition, performing relativistic many-body calculations of several atomic properties important for optical clock development. All ions discussed are …
We propose here a few selective highly charged ions (HCIs), namely Ni$^{12+}$ and Cu$^{13+}$, Pd$^{12+}$ and Ag$^{13+}$, that not only promise to be very high accurate optical clocks below $10^{-19}$ uncertainties, but also offer quality factors larger than $10^{15}$ and yet possess simple atomic structures for the experimental set-up. Moreover, these ions have strong optical magnetic-dipole (M1) transitions than the previously proposed HCI clocks. They can be used for the cooling and detection techniques. To demonstrate the projected fractional uncertainties below $10^{-19}$ level, we have es…
Recent developments in frequency metrology and optical clocks have been based on electronic transitions in atoms and singly charged ions as references. These systems have enabled relative frequency uncertainties at a level of a few parts in $10^{-18}$. This accomplishment not only allows for extremely accurate time and frequency measurements, but also to probe our understanding of fundamental physics, such as variation of fundamental constants, violation of the local Lorentz invariance, and forces beyond the Standard Model of Physics. In addition, novel clocks are driving the development of so…
Derivations for the higher tensor components of the quadrupole polarizabilities are given and their values for the metastable states of the Ca$^+$, Sr$^+$ and Ba$^+$ alkaline earth-metal ions are estimated. We also give the scalar quadrupole polarizabilities of the ground and metastable states of these ions to compare our results with the previously available theoretical and experimental results. Reasonably good agreement between our calculations with the previous values of scalar quadrupole polarizabilities demonstrate their correctness. The reported scalar and tensor quadrupole polarizabilit…
We present additional magic wavelengths ($λ_{\rm{magic}}$) for the clock transitions in the alkaline-earth metal ions considering circular polarized light aside from our previously reported values in [J. Kaur et al., Phys. Rev. A {\bf 92}, 031402(R) (2015)] for the linearly polarized light. Contributions from the vector component to the dynamic dipole polarizabilities ($α_d(ω)$) of the atomic states associated with the clock transitions play major roles in the evaluation of these $λ_{\rm{magic}}$, hence facilitating in choosing circular polarization of lasers in the experiments. Moreover, the …
Optical atomic clocks using highly-charged ions hold an intriguing promise of metrology at the 19th significant figure. Here we study transitions within the $4f^{12}$ ground-state electronic configuration of highly charged ions. We consider isotopes lacking hyperfine structure and show that the detrimental effects of coupling of electronic quadrupole moments to gradients of trapping electric field can be effectively reduced by using specially chosen virtual clock transitions. The estimated systematic fractional clock accuracy is shown to be below $10^{-19}$.
An ultra-stable optical clock based on coherent population trapping effect of alkaline-earth ions, such as Ca$^+$, Sr$^+$, Ba$^+$, is analyzed here. The proposed transitions use the odd isotopes, so that the frequency shift is insensitive to the applied magnetic field. To enhance the signal, a large number of ions are trapped in a linear Paul trap, and laser cooled to crystallize such that the ions are in the Lamb-Dicke regime to avoid first order Doppler shift. Other relevant frequency shifts are also analyzed. Further techniques to improve the stability of the clock signal are discussed.
We demonstrate that several metastable excited states in Hf$~$II, Hf$~$IV and W$~$VI ions may be good clock states since they are sufficiently long-living and are not sensitive to the perturbations. Cooling E1 transitions are available. Energy levels, Landé $g$-factors, transition amplitudes for electric dipole (E1), electric quadrupole (E2), and magnetic dipole (M1) transitions, lifetimes, and electric quadrupole moments for Hf$~$II, Hf$~$IV, and W$~$VI ions are investigated using a combination of several methods of relativistic many-body calculations including the configuration interaction (…
This paper reports the direct temperature determination of sympathetically cooled 113Cd+ ions with laser-cooled 24Mg+ in a linear Paul trap. The sympathetically cooled ion species distribute in the outer shell of the large ensembles, which contain up to 3.3E5 ions. With optimized parameters, the minimum temperature of the sympathetically cooled 113Cd+ ions was measured to be tens of mK. These results indicate promising performance for microwave atomic clocks. The second order Doppler frequency shift is two orders of magnitudes lower and the Dick effect is suppressed.
Optical clocks based on ensembles of trapped ions offer the perspective of record frequency uncertainty with good short-term stability. Most suitable atomic species lack closed transitions for fast detection such that the clock signal has to be read out indirectly through transferring the quantum state of clock ions to co-trapped logic ions by means of quantum logic operations. For ensembles of clock ions existing methods for quantum logic readout require a linear overhead in either time or the number of logic ions. Here we report a quantum algorithmic readout whose overhead scales logarithmic…
We propose a novel class of atomic clocks based on highly charged ions. We consider highly-forbidden laser-accessible transitions within the $4f^{12}$ ground-state configurations of highly charged ions. Our evaluation of systematic effects demonstrates that these transitions may be used for building exceptionally accurate atomic clocks which may compete in accuracy with recently proposed nuclear clock.
We report frequency measurement of the clock transition in an 115In+ ion sympathetically-cooled with Ca+ ions in a linear rf trap. The Ca+ ions are used as a probe of the external electromagnetic field and as the coolant for preparing the cold In+. The frequency is determined to be 1 267 402 452 901 049.9 (6.9) Hz by averaging 36 measurements using an optical frequency comb referenced to the frequency standards located in the same site.
Level crossings in the ground state of ions occur when the nuclear charge Z and ion charge Z_ion are varied along an isoelectronic sequence until the two outermost shells are nearly degenerate. We examine all available level crossings in the periodic table for both near neutral ions and highly charged ions (HCIs). Normal E1 transitions in HCIs are in X-ray range, however level crossings allow for optical electromagnetic transitions that could form the reference transition for high accuracy atomic clocks. Optical E1 (due to configuration mixing), M1 and E2 transitions are available in HCIs near…
We present an experiment to characterize our new linear ion trap designed for the operation of a many-ion optical clock using 115-In^+ as clock ions. For the characterization of the trap as well as the sympathetic cooling of the clock ions we use 172-Yb^+. The trap design has been derived from finite element method (FEM) calculations and a first prototype based on glass-reinforced thermoset laminates was built. This paper details on the trap manufacturing process and micromotion measurement. Excess micromotion is measured using photon-correlation spectroscopy with a resolution of 1.1nm in moti…
Proposal for a multi-ion optical clock with hundreds of ions
P.N. Lebedev Physical Institute of the Russian Academy of Sciences（俄罗斯科学院列别杰夫物理研究所）；Key Laboratory of Quantum State Construction and Manipulation (Ministry of Education), School of Physics, Renmin University of China（中国人民大学物理学院量子态构建与操控教育部重点实验室）；Russian Quantum Center, Skolkovo（斯科尔科沃俄罗斯量子中心）；Beijing Academy of Quantum Information Sciences（北京量子信息科学研究院）
We present the concluding result from an Ives-Stilwell-type time dilation experiment using 7Li+ ions confined at a velocity of beta = v/c = 0.338 in the storage ring ESR at Darmstadt. A Lambda-type three-level system within the hyperfine structure of the 7Li+ triplet S1-P2 line is driven by two laser beams aligned parallel and antiparallel relative to the ion beam. The lasers' Doppler shifted frequencies required for resonance are measured with an accuracy of < 4 ppb using optical-optical double resonance spectroscopy. This allows us to verify the Special Relativity relation between the time d…
We report sympathetic cooling of $^{113}$Cd$^+$ by laser-cooled $^{40}$Ca$^+$ in a linear Paul trap for microwave clocks. Long-term low-temperature confinement of $^{113}$Cd$^+$ ions was achieved. The temperature of these ions was measured at $90(10)$ mK, and the corresponding uncertainty arising from the second-order Doppler shifts was estimated to a level of $2\times10^{-17}$. Up to $4.2\times10^5$ Cd$^+$ ions were confined in the trap, and the confinement time constant was measured to be 84 hours. After three hours of confinement, there were still $10^5$ Cd$^+$ ions present, indicating that…
We present a novel method for engineering an optical clock transition that is robust against external field fluctuations and is able to overcome limits resulting from field inhomogeneities. The technique is based on the application of continuous driving fields to form a pair of dressed states essentially free of all relevant shifts. Specifically, the clock transition is robust to magnetic shifts, quadrupole and other tensor shifts, and amplitude fluctuations of the driving fields. The scheme is applicable to either a single ion or an ensemble of ions, and is relevant for several types of ions,…
We report on the design of a segmented linear Paul trap for optical clock applications using trapped ion Coulomb crystals. For an optical clock with an improved short-term stability and a fractional frequency uncertainty of 10^-18, we propose 115In+ ions sympathetically cooled by 172Yb+. We discuss the systematic frequency shifts of such a frequency standard. In particular, we elaborate on high precision calculations of the electric radiofrequency field of the ion trap using the finite element method. These calculations are used to find a scalable design with minimized excess micromotion of th…
We propose 10 highly-charged ions as candidates for the development of next generation atomic clocks, quantum information, and search for $α$-variation. They have long-lived metastable states with transition frequencies to the ground state between 170-3000 nm, relatively simple electronic structure, stable isotopes and high sensitivity to $α$-variation (e.g., Sm$^{14+}$, Pr$^{10+}$, Sm$^{13+}$, Nd$^{10+}$). We predict their properties crucial for the experimental exploration and highlight particularly attractive systems for these applications.
We studied the recollision dynamics between the electrons and D$_2^+$ ions following the tunneling ionization of D$_2$ molecules in an intense short pulse laser field. The returning electron collisionally excites the D$_2^+$ ion to excited electronic states from there D$_2^+$ can dissociate or be further ionized by the laser field, resulting in D$^+$ + D or D$^+$ + D$^+$, respectively. We modeled the fragmentation dynamics and calculated the resulting kinetic energy spectrum of D$^+$ to compare with recent experiments. Since the recollision time is locked to the tunneling ionization time which…
We study a wide range of neutral atoms and ions suitable for ultra-precise atomic optical clocks with naturally suppressed black body radiation shift of clock transition frequency. Calculations show that scalar polarizabilities of clock states cancel each other for at least one order of magnitude for considered systems. Results for calculations of frequencies, quadrupole moments of the states, clock transition amplitudes and natural widths of upper clock states are presented.
We evaluate the feasibility of using magnetic-dipole (M1) transitions in highly-charged ions as a basis of an optical atomic clockwork of exceptional accuracy. We consider a range of possibilities, including M1 transitions between clock levels of the same fine-structure and hyperfine-structure manifolds. In highly charged ions these transitions lie in the optical part of the spectra and can be probed with lasers. The most direct advantage of our proposal comes from the low degeneracy of clock levels and the simplicity of atomic structure in combination with negligible quadrupolar shift. We dem…
Recent theoretical works have proposed atomic clocks based on narrow optical transitions in highly charged ions. The most interesting candidates for searches of new physics are those which occur at rare orbital crossings where the shell structure of the periodic table is reordered. There are only three such crossings expected to be accessible in highly charged ions, and hitherto none have been observed as both experiment and theory have proven difficult. In this work we observe an orbital crossing in highly charged ions for the first time, in a system chosen to be tractable from both sides: Pr…
Attempts are made to unify gravity with the other three fundamental forces of nature. As suggested by higher dimensional models, this unification may require space and time variation of some dimensionless fundamental constants. In this scenario, probing temporal variation of the electromagnetic fine structure constant ($α= \frac{e^2} {\hbar c}$) in low energy regimes at the cosmological time scale is of immense interest. Atomic clocks are ideal candidates for probing $α$ variation because their transition frequencies are measured to ultra-high precision accuracy. Since atomic transition freque…
Optical atomic clocks represent the state-of-the-art in the frontier of modern measurement science. In this article we provide a detailed review on the development of optical atomic clocks that are based on trapped single ions and many neutral atoms. We discuss important technical ingredients for optical clocks, and we present measurement precision and systematic uncertainty associated with some of the best clocks to date. We conclude with an outlook on the exciting prospect for clock applications.
Optical lattice clocks are at the forefront of frequency metrology. Both the instability and systematic uncertainty of these clocks have been reported to be two orders of magnitude smaller than the best microwave clocks. For this reason, a redefinition of the SI second based on optical clocks seems possible in the near future. However, the operation of optical lattice clocks has not yet reached the reliability that microwave clocks have achieved so far. In this paper, we report on the operation of a strontium optical lattice clock that spans several weeks, with more than 80% uptime. We make us…
Iridium ions near $4f$-$5s$ level crossings are the leading candidates for a new type of atomic clocks with a high projected accuracy and a very high sensitivity to the temporal variation of the fine structure constant $α$. To identify spectra of these ions in experiment accurate calculations of the spectra and electromagnetic transition probabilities should be performed. Properties of the $4f$-core-excited states in Ir$^{16+}$, Ir$^{17+}$, and Ir$^{18+}$ ions are evaluated using relativistic many-body perturbation theory and Hartree-Fock-Relativistic method (COWAN code). We evaluate excitatio…
We report on the first frequency ratio measurement of an $^{115}$In+ single ion clock and a $^{87}$Sr optical lattice clock. A hydrogen maser serves as a reference oscillator to measure the ratio by independent optical combs. Over more than 90 000 seconds of measurement time, the frequency ratio $f_{\rm{In^+}}/f_{\rm{Sr}}$ is determined to be 2.952 748 749 874 863 4(21) with relative uncertainty of $7.0 \times 10^{-16}$. The measurement creates a new connection in the network of frequency ratios of optical clocks.
Collisions with background gas can perturb the transition frequency of trapped ions in an optical atomic clock. We develop a non-perturbative framework based on a quantum channel description of the scattering process, and use it to derive a master equation which leads to a simple analytic expression for the collisional frequency shift. As a demonstration of our method, we calculate the frequency shift of the Sr$^+$ optical atomic clock transition due to elastic collisions with helium.
The rapid increase in accuracy and stability of optical atomic clocks compared to the caesium atomic clock as primary standard of time and frequency asks for a future re-definition of the second in the International System of Units (SI). The status of the optical clocks based on either single ions in radio-frequency traps or on neutral atoms stored in an optical lattice is described with special emphasis of the current work at the Physikalisch-Technische Bundesanstalt (PTB). Besides the development and operation of different optical clocks with estimated fractional uncertainties in the 10^-18 …
We present an extended model for the lattice-induced light shifts of the clock frequency in optical lattice clocks, applicable to a wide range of operating conditions. The model extensions cover radial motional states with sufficient energies to invalidate the harmonic approximation of the confining potential. We reevaluate lattice-induced light shifts in our Yb optical lattice clock with an uncertainty of 6.1E-18 under typical clock operating conditions.
We study the Ho$^{14+}$ ion as a candidate for extremely accurate and stable optical atomic clock which is sensitive to the time variation of the fine structure constant. We demonstrate that the proposed system has all desired features including relatively strong optical electric dipole and magnetic dipole transitions which can be used for cooling and detection. Zero quadrupole moments for the relevant states in the clock transition allows interrogating multiple ions to improve the clock stability.
For the past 15 years, tremendous progress within the fields of laser stabilization, optical frequency combs and atom cooling and trapping have allowed the realization of optical atomic clocks with unrivaled performances. These instruments can perform frequency comparisons with fractional uncertainties well below $10^{-17}$, finding applications in fundamental physics tests, relativistic geodesy, and time and frequency metrology. Even though most optical clocks are currently laboratory setups, several proposals for using these clocks for field measurements or within an optical clock network ha…
Due to the low sensitivity of the thulium optical clock to black-body radiation and good accuracy and stability estimations, it appears to be one of the most promising transportable optical clocks. One of the leading systematic effects for Tm clock transition, namely the second-order Zeeman effect, can be canceled by probing two clock transitions between different hyperfine levels of ground and metastable states during the clock operation. We prepare the atoms in $m_F=0$ state of both ground hyperfine levels simultaneously and excite alternately two clock transitions. Here we demonstrate effic…
We develop a method of spectroscopy that uses a weak static magnetic field to enable direct optical excitation of forbidden electric-dipole transitions that are otherwise prohibitively weak. The power of this scheme is demonstrated using the important application of optical atomic clocks based on neutral atoms confined to an optical lattice. The simple experimental implementation of this method -- a single clock laser combined with a DC magnetic field-- relaxes stringent requirements in current lattice-based clocks (e.g., magnetic field shielding and light polarization), and could therefore ex…
The systematic shifts of the transition frequencies in the molecular hydrogen ions are of relevance to ultra-high-resolution radio-frequency, microwave and optical spectroscopy of these systems, performed in ion traps. We develop the ab-initio description of the interaction of the electric quadrupole moment of this class of molecules with the static electric field gradients present in ion traps. In good approximation, it is described in terms of an effective perturbation hamiltonian. An approximate treatment is then performed in the Born-Oppenheimer approximation. We give an expression of the …
We propose a new class of atomic microwave clocks based on the hyperfine transitions in the ground state of aluminum or gallium atoms trapped in optical lattices. For these elements magic wavelengths exist at which both levels of the hyperfine doublet are shifted at the same rate by the lattice laser field, cancelling its effect on the clock transition. Our analysis of various systematic effects shows that, while offering an improved control over systematic errors, the accuracy of the proposed microwave clock is competitive to that of the state-of-the-art primary frequency standard.
Black-body radiation (BBR) shifts of $^3\!P_0-^1\!S_0$ clock transition in divalent atoms Cd and Zn are evaluated using accurate relativistic many-body techniques of atomic structure. Static polarizabilities of the clock levels and relevant electric-dipole matrix elements are computed. We also present a comparative overview of the BBR shifts in optical clocks based on neutral divalent atoms trapped in optical lattices.
We carried out detailed high-precision study of Ag-like Nd$^{13+}$, Sm$^{15+}$ and In-like Ce$^{9+}$, Pr$^{10+}$, Nd$^{11+}$, Sm$^{13+}$, Eu$^{14+}$ highly-charged ions. These ions were identified to be of particular interest to the development of ultra-accurate atomic clocks, search for variation of the fine-structure constant $α$, and quantum information [Safronova et. al. Phys. Rev. Lett. 113, 030801 (2014)]. Relativistic linearized coupled-cluster method was used for Ag-like ion calculations, and a hybrid approach that combines configuration interaction and a variant of the coupled-cluster…
We demonstrate state-of-the-art technique of an active clock to provide a continuous superradiant lasing signal using an ensemble of trapped Cs atoms in the optical lattice. A magic wavelength of the proposed |7S1/2; F = 4, MF = 0> - |6P3/2; F = 3, MF = 0> clock transition in Cs atom is identified at 1181 nm for constructing the optical lattice. Pertinent optical lines are also found for pumping and repumping atoms from their ground states. A fractional uncertainty about 10-15 level to the clock frequency has been predicted by carrying out rigorous calculations of several atomic properties. Th…
We report on a transportable optical clock, based on laser-cooled strontium atoms trapped in an optical lattice. The experimental apparatus is composed of a compact source of ultra-cold strontium atoms including a compact cooling laser set-up and a transportable ultra-stable laser for interrogating the optical clock transition. The whole setup (excluding electronics) fits within a volume of less than 2 m$^3$. The high degree of operation reliability of both systems allowed the spectroscopy of the clock transition to be performed with 10 Hz resolution. We estimate an uncertainty of the clock of…
A Wannier-Stark optical lattice clock has demonstrated unprecedented measurement precision for optical atomic clocks. We present a systematic evaluation of the lattice light shift, a necessary next step for establishing this system as an accurate atomic clock. With precise control of the atomic motional states in the lattice, we report accurate measurements of the multipolar and the hyperpolar contributions and the operational lattice light shift with a fractional frequency uncertainty of 3.5$\times$10${}^{-19}$.
We have developed an optical lattice clock that can operate in dual modes: a strontium (Sr) clock mode and an ytterbium (Yb) clock mode. Dual-mode operation of the Sr-Yb optical lattice clock is achieved by alternately cooling and trapping $^{87}$Sr and $^{171}$Yb atoms inside the vacuum chamber of the clock. Optical lattices for Sr and Yb atoms were arranged with horizontal and vertical configurations, respectively, resulting in a small distance of the order of 100 $μ$m between the trapped Sr and Yb atoms. The $^{1}$S$_{0}$-$^{3}$P$_{0}$ clock transitions in the trapped atoms were interrogate…
