Precision spectroscopy on cold molecules can potentially enable novel tests of fundamental laws of physics and alternative determination of some fundamental constants. Realizing this potential requires a thorough understanding of the systematic effects that shift the energy levels of molecules. We have performed a complete ab initio calculation of the magnetic field effects for a particular system, the heteronuclear molecular hydrogen ion HD+. Different spectroscopic schemes have been considered, and numerous transitions, all accessible by modern radiation sources and exhibiting well controllable or negligible Zeeman shift, have been found to exist. Thus, HD+ is a perspective candidate for determination of the ratio of electron-to-nuclear reduced mass, and for tests of its time-independence.
We report the evaluation of the second order Zeeman shift in the continuous atomic fountain clock FoCS-2. Because of the continuous operation and of its geometrical constraints, the methods used in pulsed fountains are not applicable. We use here time-resolved Zeeman spectroscopy to probe the magnetic field profile in the clock. The pulses of ac magnetic excitation allow us to spatially resolve the Zeeman frequency and to evaluate the Zeeman shift with a relative uncertainty smaller than 10E-16.
We present an experimental concept and setup for laser-microwave double-resonance spectroscopy of highly charged ions in a Penning trap. Such spectroscopy allows a highly precise measurement of the Zeeman splittings of fine- and hyperfine-structure levels due the magnetic field of the trap. We have performed detailed calculations of the Zeeman effect in the framework of quantum electrodynamics of bound states as present in such highly charged ions. We find that apart from the linear Zeeman effect, second- and third-order Zeeman effects also contribute to the splittings on a level of 10^-4 and …
Relativistic calculations of the second- and third-order contributions in magnetic field to the Zeeman splitting in boronlike ions are presented for the wide range of nuclear charge numbers $Z=6$--$92$. The interelectronic-interaction correction of the first order in $1/Z$ is evaluated to all orders in $αZ$. The higher-order corrections in $1/Z$ are taken into account approximately by means of effective screening potentials. The obtained results are important for interpretation of experimental data on the Zeeman splitting in boronlike ions, in particular, for the ARTEMIS experiment presently i…
Characterization of rf field-induced a.c. Zeeman shift in multi-level highly charged ions
Physikalisch-Technische Bundesanstalt（德国联邦物理技术研究院）；Max-Planck-Institut für Kernphysik（马克斯·普朗克核物理研究所）；Institut für Quantenoptik, Leibniz Universität Hannover（汉诺威莱布尼茨大学量子光学研究所）
Zeeman spectroscopy is used to demonstrate that phenomenological crystal-field parameters determined for the two $C_1$ point-group sites in Er$^{3+}$:Y$_2$SiO$_5$ may be transferred to other ions. The two crystallographic six- and seven-coordinate substitutional sites may be distinguished by comparing the spectra with crystal-field calculations.
Rotational levels of molecular free radicals can be tuned to degeneracy using laboratory-scale magnetic fields. Because of their intrinsically narrow width, these level crossings of opposite-parity states have been proposed for use in the study of parity-violating interactions and other applications. We experimentally study a typical manifestation of this system using $^{138}$BaF. Using a Stark-mixing method for detection, we demonstrate level-crossing signals with spectral width as small as 6 kHz. We use our data to verify the predicted lineshapes, transition dipole moments, and Stark shifts,…
The fully relativistic theory of the Zeeman splitting of the $1s$ hyperfine structure levels in hydrogenlike ions is considered for the magnetic field magnitude in the range from 1 to 10 T. The second-order corrections to the Breit -- Rabi formula are calculated and discussed. The results can be used for a precise determination of nuclear magnetic moments from $g$ factor experiments.
ITMO University（ITMO大学）；HSE University（高等经济大学）；Petersburg Nuclear Physics Institute named by B. P. Konstantinov of National Research Centre “Kurchatov Institute”（国立核子研究中心“库尔恰托夫研究所”鲍·彼·康斯坦丁诺夫圣彼得堡核物理研究所）；St. Petersburg State University（圣彼得堡国立大学）
High-resolution Zeeman spectroscopy of electronic-nuclear hyperfine levels of ${^5\mathrm{I}_8}\rightarrow{^5\mathrm{I}_7}$ transitions in Ho$^{3+}$:Y$_2$SiO$_5$ is reported. Crystal-field parameters determined for the two $C_1$ symmetry sites in Er$^{3+}$:Y$_2$SiO$_5$ are successfully used to model the Zeeman-hyperfine data, including the prediction of avoided crossings between hyperfine levels under the influence of an external magnetic field. The two six- and seven-coordinate substitutional sites may be distinguished by comparing the spectra with crystal-field calculations.
We present a quantum logic scheme to detect atomic and molecular ions in different states of angular momentum based on their magnetic $g$-factors. The state-dependent magnetic $g$-factors mean that electronic, rotational or hyperfine states may be distinguished by their Zeeman splittings in a given magnetic field. Driving motional sidebands of a chosen Zeeman splitting enables reading out the corresponding state of angular momentum with an auxillary logic ion. As a proof-of-principle demonstration, we show that we can detect the ground electronic state of a ${^{174}}$Yb$^+$ ion using ${^{171}}…
We present a general discussion of the techniques of destabilizing dark states in laser-driven atoms with either a magnetic field or modulated laser polarization. We show that the photon scattering rate is maximized at a particular evolution rate of the dark state. We also find that the atomic resonance curve is significantly broadened when the evolution rate is far from this optimum value. These results are illustrated with detailed examples of destabilizing dark states in some commonly-trapped ions and supported by insights derived from numerical calculations and simple theoretical models.
We report an improved measurement of the Landé g factor of the 5D5/2 state of singly ionized barium. Measurements were performed on single Doppler-cooled 138Ba+ ions in linear Paul traps using two similar, independent apparatuses. Transitions between Zeeman sublevels of the 6S1/2 and 5D5/2 states were driven with two independent, stabilized radio-frequency synthesizers using a dedicated electrode within each ion trap chamber. State detection within each Zeeman manifold was achieved with a frequency-stabilized fiber laser operating at 1.76 microns. By calculating the ratio of the two Zeeman spl…
The fully relativistic theory of the Zeeman splitting of the $(1s)^2 2s$ hyperfine-structure levels in lithiumlike ions with $Z=6 - 32$ is considered for the magnetic field magnitude in the range from 1 to 10 T. The second-order corrections to the Breit -- Rabi formula are calculated and discussed including the one-electron contributions as well as the interelectronic-interaction effects of order 1/Z. The 1/Z corrections are evaluated within a rigorous QED approach. These corrections are combined with other interelectronic-interaction, QED, nuclear recoil, and nuclear size corrections to obtai…
We present the results of an experimental and theoretical study of the electronically excited $\tripletex$ state of $^{87}$Rb$_2$ molecules. The vibrational energies are measured for deeply bound states from the bottom up to $v'=15$ using laser spectroscopy of ultracold Rb$_2$ Feshbach molecules. The spectrum of each vibrational state is dominated by a 47\,GHz splitting into a $\cog$ and $\clg$ component caused mainly by a strong second order spin-orbit interaction. Our spectroscopy fully resolves the rotational, hyperfine, and Zeeman structure of the spectrum. We are able to describe to first…
Motional ground state cooling and internal state preparation are important elements for quantum logic spectroscopy (QLS), a class of quantum information processing. Since QLS does not require the high gate fidelities usually associated with quantum computation and quantum simulation, it is possible to make simplifying choices in ion species and quantum protocols at the expense of some fidelity. Here, we report sideband cooling and motional state detection protocols for $^{138}$Ba$^+$ of sufficient fidelity for QLS without an extremely narrowband laser or the use of a species with hyperfine str…
Active frequency stabilization of a laser to an atomic or molecular resonance underpins many modern-day AMO physics experiments. With a flat background and high signal-to-noise ratio, modulation transfer spectroscopy (MTS) offers an accurate and stable method for laser locking. Despite its benefits, however, the four-wave mixing process that is inherent to the MTS technique entails that the strongest modulation transfer signals are only observed for closed transitions, excluding MTS from numerous applications. Here, we report for the first time the observation of a magnetically tunable MTS err…
We propose a high-performance atomic clock based on the 1.81 PHz transition between the ground and first-excited state of doubly ionized lead. Utilizing an even isotope of lead, both clock states have $I=J=F=0$, where $I$, $J$, and $F$ are the conventional quantum numbers specifying nuclear, electronic, and total angular momentum, respectively. The clock states are nondegenerate and completely immune to nonscalar perturbations, including first order Zeeman and electric quadrupole shifts. Additionally, the proposed clock is relatively insusceptible to other frequency shifts (blackbody radiation…
With the development of microwave atomic clocks, the Zeeman shifts for the spectral lines of black-body radiation need to be investigated carefully. In this Letter, the frequency shifts of hyperfine splittings of atomic ground states due to the magnetic field of black-body radiation are reported. The relative frequency shifts of different alkali atoms and alkali-like ions, which could be candidates of microwave atomic clocks, were calculated. The results vary from $-0.977\times10^{-17}[T(K)/300]^{2}$ to $-1.947\times10^{-17}[T(K)/300]^{2}$ for different atoms considered. These results are cons…
We perform Zeeman spectroscopy on a Rydberg electromagnetically induced transparency (EIT) system in a room-temperature Cs vapor cell, in magnetic fields up to 50~Gauss and for several polarization configurations. The magnetic interactions of the $\vert 6S_{1/2}, F_g=4 \rangle$ ground, $\vert 6P_{3/2}, F_e=5 \rangle$ intermediate, and $\vert 33S_{1/2} \rangle$ Rydberg states that form the ladder-type EIT system are in the linear Zeeman, quadratic Zeeman, and the deep hyperfine Paschen-Back regimes, respectively. Starting in magnetic fields of about 5~Gauss, the spectra develop an asymmetry tha…
We use the dressed atom formalism to calculate the frequency shift in a hydrogen maser induced by applied radiation near the Zeeman frequency, and find excellent agreement with a previous calculation made in the bare atom basis. The maser oscillates on the Delta_F = 1, Delta_m_F = 0 hyperfine transition, while the applied field is swept through the F = 1, Delta_m_F = \pm 1 Zeeman resonance. We determine the effect of the applied field on the Zeeman levels using the dressed atom picture, and then calculate the maser frequency shift by coupling the dressed states to the microwave cavity. Qualita…
Multipole radiofrequency ion traps are a highly versatile tool to study molecular ions and their interactions in a well-controllable environment. In particular the cryogenic 22-pole ion trap configuration is used to study ion-molecule reactions and complex molecular spectroscopy at temperatures between few Kelvin and room temperatures. This article presents a tutorial on radiofrequency ion trapping in multipole electrode configurations. Stable trapping conditions and buffer gas cooling, as well as important heating mechanisms, are discussed. In addition, selected experimental studies on cation…
Metastable helium molecules (He$_2^*$) have been generated by striking a discharge in a supersonic expansion of helium gas from a pulsed valve. When operating the pulsed valve at room temperature, 77K, and 10K, the mean velocity of the supersonic beam was measured to be 1900m/s, 980m/s, and 530m/s, respectively. A 55-stage Zeeman decelerator operated in a phase-stable manner was then used to further reduce the beam velocity and tune it in the range between 100 and 150m/s. The internal-state distribution of the decelerated sample was established by photoionization spectroscopy.
A general method for rotational microwave spectroscopy and control of polar molecular ions via direct microwave addressing is considered. Our method makes use of spatially varying AC Stark shifts, induced by far off-resonant, focused laser beams to achieve an effective coupling between the rotational state of a molecular ion and the electronic state of an atomic ion. In this setting, the atomic ion is used for read-out of the molecular ion state, in a manner analogous to quantum logic spectroscopy based on Raman transitions. In addition to high-precision spectroscopy, this setting allows for r…
We study the combination of hyperfine and Zeeman structure in the spin-orbit coupled $A^1Σ_u^+-b^3Π_u$ complex of $^{87}\textrm{Rb}_2$. For this purpose, absorption spectroscopy at a magnetic field around $B=1000\:\textrm{G}$ is carried out. We drive optical dipole transitions from the lowest rotational state of an ultracold Feshbach molecule to various vibrational levels with $0^+$ symmetry of the $A-b$ complex. In contrast to previous measurements with rotationally excited alkali-dimers, we do not observe equal spacings of the hyperfine levels. In addition, the spectra vary substantially for…
We examine the effect of a parasitic rf magnetic field, attributed to ion trapping, on the highly anticipated nuclear clock based on $^{229}$Th$^{3+}$ [C. J. Campbell et al., Phys. Rev. Lett. 108, 120802 (2012)]. The rf magnetic field induces an ac Zeeman shift to the clock frequency. As we demonstrate, this shift threatens to be the dominant systematic frequency shift for the clock, exceeding other systematic frequency shifts and the projected systematic uncertainty of the clock by orders of magnitude. We propose practical means to suppress or eliminate this shift.
A cryogenic radio-frequency ion trap system designed for quantum logic spectroscopy of highly charged ions is presented. It includes a segmented linear Paul trap, an in-vacuum imaging lens and a helical resonator. We demonstrate ground state cooling of all three modes of motion of a single $^9$Be$^+$ ion and determine their heating rates as well as excess axial micromotion. The trap shows one of the lowest levels of electric field noise published to date. We investigate the magnetic-field noise suppression in cryogenic shields made from segmented copper, the resulting magnetic field stability …
We review recent experiments on HD$^+$ spectroscopy. The reduced proton-deuteron mass to electron mass ratio, $μ_{pd}/m_e$, is inferred from the comparison of theory and experiment. Theoretical issues related to the calculations of the spin structure, which are currently the main limiting factor of theoretical accuracy, are discussed.
We have conceived, built and operated a 'half-open' cylindrical Penning trap for the confinement and laser spectroscopy of highly charged ions. This trap allows fluorescence detection employing a solid angle which is about one order of magnitude larger than in conventional cylindrical Penning traps. At the same time, the desired electrostatic and magnetostatic properties of a closed-endcap cylindrical Penning trap are preserved in this congfiuration. We give a detailed account on the design and confinement properties, a characterization of the trap and show first results of light collection wi…
The coupled motion of ions in a radiofrequency trap has been used to connect the frequency- dependent laser-induced heating of a sympathetically cooled spectroscopy ion with changes in the fluorescence of a laser-cooled control ion. This technique, sympathetic heating spectroscopy, is demonstrated using two isotopes of calcium. In the experiment, a few scattered photons from the spectroscopy ion are transformed into a large deviation from the steady-state fluorescence of the control ion. This allows us to detect an optical transition where the number of scattered photons is below our fluoresce…
We experimentally re-evaluate the fine structure of Sn$^{11+...14+}$ ions. These ions are essential in bright extreme-ultraviolet (EUV) plasma-light sources for next-generation nanolithography, but their complex electronic structure is an open challenge for both theory and experiment. We combine optical spectroscopy of magnetic dipole $M1$ transitions, in a wavelength range covering 260\,nm to 780\,nm, with charge-state selective ionization in an electron beam ion trap. Our measurements confirm the predictive power of \emph{ab initio} calculations based on Fock space coupled cluster theory. We…
In this paper we present a technique for the precise measurement of electric dipole allowed transitions in trapped ions. By applying a probe and a cooling laser in quick succession, the full transition can be probed without causing distortion from heating the ion. In addition, two probes can be utilized to measure a dispersion-like signal, which is well suited to stabilizing the laser to the transition. We have fully characterized the parameters for the measurement and find that it is possible to measure the transition frequency to better than 100kHz with an interrogation time of 30s. The long…
We describe the current status of high-precision ab initio calculations of the spectra of molecular hydrogen ions (H_2^+ and HD^+) and of two experiments for vibrational spectroscopy. The perspectives for a comparison between theory and experiment at a level of 1 ppb are considered.
We present extreme ultraviolet and visible spectra of promethiumlike tungsten and gold obtained with an electron beam ion trap (EBIT). Although the contributions from a few charge states are involved in the spectra, the charge state of the ion assigned to the observed lines is definitely identified by the time-of-flight analysis of the ions performed at the same time with the spectroscopic measurements. Experimental results are compared with collisional-radiative model calculations as well as previous experimental and theoretical studies.
Precisely evaluating the systematic error induced by the quadratic Zeeman effect is important for developing atom interferometer gravimeters aiming at an accuracy in the regime ( ). This paper reports on the experimental investigation of Raman spectroscopy-based magnetic field measurements and the evaluation of the systematic error in the Gravimetric Atom Interferometer (GAIN) due to quadratic Zeeman effect. We discuss Raman duration and frequency step size dependent magnetic field measurement uncertainty, present vector light shift (VLS) and tensor light shift (TLS) induced magnetic field mea…
We have extended Ramsey spectroscopy by stepping the probe frequency during the two Ramsey excitation pulses to compensate frequency shifts induced by the excitation itself. This makes precision Ramsey spectroscopy applicable even for transitions that have Stark and Zeeman shifts comparable to the spectroscopic resolution. The method enables a new way to evaluate and compensate key frequency shifts, which benefits in particular, optical clocks based on magnetic field-induced, spectroscopy, two-photon transitions, or heavily forbidden transitions.
Engineering magnetically insensitive qubits in metastable electronic D-states of trapped ions
IonQ, Inc.（IonQ公司）；Joint Quantum Institute and Department of Physics, University of Maryland（马里兰大学联合量子研究所与物理系）；Infleqtion, Inc.（Infleqtion公司）；National Institute of Standards and Technology（美国国家标准与技术研究院）；Keysight Technologies（是德科技）；Duke Quantum Center, Department of Electrical and Computer Engineering and Department of Physics, Duke University（杜克大学电气与计算机工程系、物理系及杜克量子中心）
We investigate the interplay between Zeeman and light shifts in the transmission spectrum of an optically trapped, spin-polarized Rubidium atom. The spectral shape of the transmission changes from multiple, broad resonances to a single, narrow Lorentzian with a high resonant extinction value when we increase the magnetic field strength and lower the depth of the dipole trap. We present an experimental configuration well-suited for quantum information applications in that it enables not only efficient light-atom coupling but also a long coherence time between ground state hyperfine levels.
We devise a perturbation-immune version of Ramsey's method of separated oscillatory fields. Spectroscopy of an atomic clock transition without compromising the clock's accuracy is accomplished by actively balancing the spectroscopic responses from phase-congruent Ramsey probe cycles of unequal durations. Our simple and universal approach eliminates a wide variety of interrogation-induced line shifts often encountered in high precision spectroscopy, among them, in particular, light shifts, phase chirps, and transient Zeeman shifts. We experimentally demonstrate auto-balanced Ramsey spectroscopy…
We consider the application of a basic principle of quantum theory, the tracelessness of a certain class of hamiltonians, to the precision spectroscopy of the molecular hydrogen ions. We show that it is possible to obtain the spin-averaged transition frequencies between states from a simple weighted sum of experimentally accessible spin-dependent transition frequencies. We discuss the cases ${\rm H}_{2}^{+}$ and ${\rm HD}^{+}$, which are distinct in the multipole character of their rovibrational transitions. Inclusion of additional frequencies permits canceling also the electric quadrupole shi…
A mixed-species geometric phase gate has been proposed for implementing quantum logic spectroscopy on trapped ions that combines probe and information transfer from the spectroscopy to the logic ion in a single pulse. We experimentally realize this method, show how it can be applied as a technique for identifying transitions in currently intractable atoms or molecules, demonstrate its reduced temperature sensitivity, and observe quantum-enhanced frequency sensitivity when it is applied to multi-ion chains. Potential applications include improved readout of trapped-ion clocks and simplified err…
An overview is presented of laser spectroscopy experiments with cold, trapped, highly-charged ions, which will be performed at the HITRAP facility at GSI in Darmstadt (Germany). These high-resolution measurements of ground state hyperfine splittings will be three orders of magnitude more precise than previous measurements. Moreover, from a comparison of measurements of the hyperfine splittings in hydrogen- and lithium-like ions of the same isotope, QED effects at high electromagnetic fields can be determined within a few percent. Several candidate ions suited for these laser spectroscopy studi…
We demonstrated a polarization-resolved high resolution spectroscopy of a visible emission line of highly charged tungsten ions (λ0 = 668.899 nm, Shinohara et al Phys. Scr. 90 125402) for the large helical device (LHD) plasma, where the tungsten ions were introduced by a pellet injection. Its spectral profile shows broadening and polarization dependence, which are attributed to the Doppler and Zeeman effects, respectively. The tungsten ion temperature was evaluated for the first time from the broadening of visible the emission line, with its emission location determined by the Abel inversion o…
We perform laser spectroscopy of Yb+ ions on the 4f14 6s 2S_{1/2} - 4f13 5d 6s 3D[3/2]_{1/2} transition at 297 nm. The frequency measurements for 170Yb+, 172Yb+, 174Yb+, and 176Yb+ reveal the specific mass shift as well as the field shifts. In addition, we demonstrate laser cooling of Yb+ ions using this transition and show that light at 297 nm can be used as the second step in the photoionization of neutral Yb atoms.
Sympathetic cooling of trapped ions has become an indispensable tool for quantum information processing and precision spectroscopy. In the simplest situation a single Doppler-cooled ion sympathetically cools another ion which typically has a different mass. We analytically investigate the effect of the mass ratio of such an ion crystal on the achievable temperature limit in the presence of external heating. As an example, we show that cooling of a single Al+ with Be+, Mg+ and Ca+ ions provides similar results for heating rates typically observed in ion traps, whereas cooling ions with a larger…
Optical spectroscopy in the gas phase is a key tool to elucidate the structure of atoms and molecules and of their interaction with external fields. The line resolution is usually limited by a combination of first-order Doppler broadening due to particle thermal motion and of a short transit time through the excitation beam. For trapped particles, suitable laser cooling techniques can lead to strong confinement (Lamb-Dicke regime, LDR) and thus to optical spectroscopy free of these effects. For non-laser coolable spectroscopy ions, this has so far only been achieved when trapping one or two at…
