The hyperfine structure of atoms and ions is widely used in fundamental and applied research. Accurate knowledge of hyperfine splitting values is essential for quantum metrology applications as well as for improving the performance of systems designed for quantum computing and simulation. We present refined values of the hyperfine splitting frequencies of the ground and clock states of thulium atom, $f_{g}^\textrm{HFS}=1\,496\,550\,658.23(3)$\,Hz and $f_{c}^\textrm{HFS}=2\,113\,946\,873.08(9)$\,Hz, respectively. The measurements are performed on an ultracold atomic ensemble in an optical lattice using combined microwave and optical transition spectroscopy. Our results improve the accuracy by 2 and 7 orders of magnitude for $f_{g}^\textrm{HFS}$ and $f_{c}^\textrm{HFS}$, respectively, compared to the previously published values. We also refine the value of the Landé g-factor of the clock level to $g_c = 0.85479(11)$.
The spectra emitted by a thulium hollow-cathode discharge lamp with argon or neon as inert gases have been recorded with a Bruker IFS 125 HR Fourier Transform spectrometer in the visible wavelength region from 400 nm to 700 nm. The paper presents the investigation of the hyperfine-structure splitting of 50 spectral lines of neutral thulium. As a result, the magnetic dipole hyperfine structure constant A for 20 fine structure levels of Tm I have been determined for the first time.
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…
Recently, the thulium atom was cooled down to the Bose-Einstein condensation temperature, thus opening a pathway to quantum simulation with this atom. However, successful simulations require instruments to control and readout states of the atom as well as the ability to control the interaction between either different species or different states of the same type of species. In this paper, we provide an experimental demonstration of high-fidelity (over 93%) manipulation of the ground state magnetic sublevels of thulium, which utilizes a simple and efficient design of a microwave (MW) antenna. T…
In this study, we investigated the hyperfine structure of 43 spectral lines of atomic thulium. We analyzed Fourier-transform spectra in the wavelength range from 700 nm to 2250 nm, which corresponds to the wavenumber range from 14300 cm-1 to 4440 cm-1, respectively. The excited thulium atoms were generated in a hollow-cathode lamp. As a result of this investigation, the magnetic-dipole hyperfine constant A of 17 fine structure levels have been determined experimentally, 14 of them for the first time. The magnetic-dipole hyperfine constant values of the three remaining levels, reported in the l…
Thulium atoms are trapped in a magneto-optical trap using a strong transition at 410 nm with a small branching ratio. We trap up to $7\times10^{4}$ atoms at a temperature of 0.8(2) mK after deceleration in a 40 cm long Zeeman slower. Optical leaks from the cooling cycle influence the lifetime of atoms in the MOT which varies between 0.3 -1.5 s in our experiments. The lower limit for the leaking rate from the upper cooling level is measured to be 22(6) s$^{-1}$. The repumping laser transferring the atomic population out of the F=3 hyperfine ground-state sublevel gives a 30% increase for the lif…
Using a newly developed laser-microwave-laser resonance method, we observed a pair of microwave transitions between hyperfine levels of the $(n,L)=(37,35)$ state of antiprotonic helium. This experiment confirms the quadruplet hyperfine structure due to the interaction of the antiproton orbital angular momentum, the electron spin and the antiproton spin as predicted by Bakalov and Korobov. The measured frequencies of $ν_{\text HF}^+ =12.89596 \pm 0.00034$ GHz and $ν_{\text HF}^- =12.92467 \pm 0.00029$ GHz agree with recent theoretical calculations on a level of $ 6 \times10^{-5}$.
Regarding trapped-ion microwave-frequency standards, we report on the determination of hyperfine splittings and Landé $g_J$ factors of $^{111,113}$Cd$^+$. The hyperfine splittings of the $5p~^2P_{3/2}$ state of $^{111,113}$Cd$^+$ ions were measured using laser-induced fluorescence spectroscopy. The Cd$^+$ ions were confined in a linear Paul trap and sympathetically cooled by Ca$^+$ ions. Furthermore, the hyperfine splittings and Landé $g_J$ factors of the $5s~^2S_{1/2}$ and $5p~^2P_{1/2,3/2}$ levels of $^{111,113}$Cd$^+$ were calculated with greater accuracy using the multiconfiguration Dirac-…
The hyperfine structure of the ground state of erbium doped yttrium orthosilicate is analyzed with the use of electron paramagnetic resonance experiments in a tunable microwave resonator. This work was prompted by the disagreement between the measurements made in zero magnetic field [Phys. Rev. B, 94, 075117, (2016)] and a previously published spin Hamiltonian, which is derived from standard EPR measurements at 9.5 GHz [Phys. Rev. B, 74, 214409, (2006)]. The ability to vary magnetic field strength, resonator frequency, and the orientation of our sample enabled us to monitor how the frequencies…
Using recently developed version of the configuration interaction method for atoms with open shells we calculate electron structure and spectroscopic properties of the mendelevium atom (Md, $Z=101$). These include energy levels, first and second ionisation potentials, electron affinity, hyperfine structure and electric dipole transition amplitudes between ground and low lying states of opposite parity. The accuracy of the calculations is controlled by performing similar calculations for lighter analog of mendelevium, thulium atom and comparing the results with experiment and other calculations…
In this work we describe the latest results for the measurements of the hyperfine structure of antiprotonic helium-3. Two out of four measurable super-super-hyperfine SSHF transition lines of the (n,L)=(36,34) state of antiprotonic helium-3 were observed. The measured frequencies of the individual transitions are 11.12548(08) GHz and 11.15793(13) GHz, with an increased precision of about 43% and 25% respectively compared to our first measurements with antiprotonic helium-3 [S. Friedreich et al., Phys. Lett. B 700 (2011) 1--6]. They are less than 0.5 MHz higher with respect to the most recent t…
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.
We identify a potential means to extract the $^{229g}$Th $\rightarrow$ $^{229m}$Th nuclear excitation energy from precision microwave spectroscopy of the $5F_{5/2,7/2}$ hyperfine manifolds in the ion $^{229g}$Th$^{3+}$. The hyperfine interaction mixes this ground fine structure doublet with states of the nuclear isomer, introducing small but observable shifts to the hyperfine sub-levels. We demonstrate how accurate atomic structure calculations may be combined with measurement of the hyperfine intervals to quantify the effects of this mixing. Further knowledge of the magnetic dipole decay rate…
Collisions with chemically inert atoms or molecules change the hyperfine coupling of an alkali-metal atom through the hyperfine-shift interaction. This interaction is responsible for the pressure shifts of the microwave resonances of alkali-metal atoms in buffer gases, is an important spin interaction in alkali-metal--noble-gas van der Waals molecules, and is anticipated to enable the magnetoassociation of ultracold molecules such as RbSr. An improved estimate is presented for the long-range asymptote of this interaction for Na, K, Rb, and Cs. To test the results, the change in hyperfine coupl…
The MuSEUM collaboration is planning measurements of the ground-state hyperfine structure (HFS) of muonium at the Japan Proton Accelerator Research Complex (J-PARC), Materials and Life Science Experimental Facility. The high-intensity beam that will soon be available at H-line allows for more precise measurements by one order of magnitude. We plan to conduct two staged measurements. First, we will measure the Mu-HFS in a near-zero magnetic field, and thereafter we will measure it in a strong magnetic field. We have developed two microwave cavities for this purpose. Furthermore, we evaluated sy…
We apply relativistic many-body methods to compute static differential polarizabilities for transitions inside the ground-state hyperfine manifolds of monovalent atoms and ions. Knowing this transition polarizability is required in a number of high-precision experiments, such as microwave atomic clocks and searches for CP-violating permanent electric dipole moments. While the traditional polarizability arises in the second-order of interaction with the externally-applied electric field, the differential polarizability involves additional contribution from the hyperfine interaction of atomic el…
The microwave clock frequency of the $|5s~^2S_{1/2}, F=0,m_F=0 \rangle \leftrightarrow |5s~^2S_{1/2}, F=1,m_F=0 \rangle$ transition in the $^{113}$Cd$^+$ ion has been reported as 15199862855.0192(10) Hz [Opt. Lett. {\bf 40}, 4249 (2015)]. Fractional systematic due to the black-body radiation (BBR) shift ($β$) arising from the Stark effect in the above clock transition was used as $-1.1 \times 10^{-16}$ from our unpublished preliminary estimation. We present here a precise value as $β=-1.815(77) \times 10^{-16}$ by carrying out rigorous calculations of third-order polarizabilities of the hyperf…
Spherically-symmetric ground states of alkali-metal atoms do not posses electric quadrupole moments. However, the hyperfine interaction between nuclear moments and atomic electrons distorts the spherical symmetry of electronic clouds and leads to non-vanishing atomic quadrupole moments. We evaluate these hyperfine-induced quadrupole moments using techniques of relativistic many-body theory and compile results for Li, Na, K, Rb, and Cs atoms. For heavy atoms we find that the hyperfine-induced quadrupole moments are strongly (two orders of magnitude) enhanced by correlation effects. We further a…
We show that the relative effect of variation of the fine structure constant in microwave transitions between very close and narrow rotational-hyperfine levels may be enhanced 2-3 orders of magnitude in diatomic molecules like LaS, LaO, LuS, YbF, etc. The enhancement is a result of cancellation between the hyperfine and rotational intervals.
The microwave resonant frequencies of ground-state 87Rb and 133Cs atoms in Xe buffer gas are shown to have a relatively large nonlinear dependence on the Xe pressure, presumably because of RbXe or CsXe van der Waals molecules. The nonlinear shifts for Xe are opposite in sign to the previously measured shifts for Ar and Kr, even though all three gases have negative linear shifts. The Xe data show striking discrepancies with the previous theory for nonlinear shifts. Most of this discrepancy is eliminated by accounting for the spin-rotation interaction in addition to the hyperfine-shift interacti…
We demonstrate coherent microwave control of rotational and hyperfine states of trapped, ultracold, and chemically stable $^{23}$Na$^{40}$K molecules. Starting with all molecules in the absolute rovibrational and hyperfine ground state, we study rotational transitions in combined magnetic and electric fields and explain the rich hyperfine structure. Following the transfer of the entire molecular ensemble into a single hyperfine level of the first rotationally excited state, $J{=}1$, we observe collisional lifetimes of more than $3\, \rm s$, comparable to those in the rovibrational ground state…
We demonstrate coherent control of both the rotational and hyperfine state of ultracold, chemically stable $^{87}$Rb$^{133}$Cs molecules with external microwave fields. We create a sample of ~2000 molecules in the lowest hyperfine level of the rovibronic ground state N = 0. We measure the transition frequencies to 8 different hyperfine levels of the N = 1 state at two magnetic fields ~23 G apart. We determine accurate values of rotational and hyperfine coupling constants that agree well with previous calculations. We observe Rabi oscillations on each transition, allowing complete population tr…
The antihydrogen programme of the ASACUSA collaboration at the antiproton decelerator of CERN focuses on Rabi-type measurements of the ground-state hyperfine splitting of antihydrogen for a test of the combined Charge-Parity-Time symmetry. The spectroscopy apparatus consists of a microwave cavity to drive hyperfine transitions and a superconducting sextupole magnet for quantum state analysis via Stern-Gerlach separation. However, the small production rates of antihydrogen forestall comprehensive performance studies on the spectroscopy apparatus. For this purpose a hydrogen source and detector …
We describe a new method to determine the position of the atomic cloud during its interaction with the microwave field in the cavity of a fountain clock. The positional information is extracted from the spectrum of the F=3,mF=0 to F=4,mF=-1 hyperfine transition, which shows a position dependent asymmetry when the magnetic C-field is tilted by a few degrees with respect to the cavity axis. Analysis of this spectral asymmetry provides the horizontal center-of-mass position for the ensemble of atoms contributing to frequency measurements. With an uncertainty on the order of 0.1 mm, the obtained i…
The sensitivity of the PbF molecule to the electron electric dipole moment has motivated detailed microwave spectroscopy. Previous theoretical approaches cannot fully explain the spectra. In turn, the explanation from "first principles" is very important both for molecular theory and for confirmation of the correctness of the interpretation of experimental data obtained with high precision. All of these issues are decisively addressed here. We have determined centrifugal correction parameters for hyperfine structure constants, both on lead and fluorine nuclei, of the $X^2Π_{1/2}$ state of lead…
Using laser optical pumping, widths and frequency shifts are determined for microwave transitions between ground-state hyperfine components of $^{85}$Rb and $^{87}$Rb atoms contained in vapor cells with alkane anti-relaxation coatings. The results are compared with data on Zeeman relaxation obtained in nonlinear magneto-optical rotation (NMOR) experiments, a comparison important for quantitative understanding of spin-relaxation mechanisms in coated cells. By comparing cells manufactured over a forty-year period we demonstrate the long-term stability of coated cells, an important property for a…
We report the initial results from a systematic study of the hyperfine (HF) structure of antiprotonic helium (n,l) = (37,~35) carried out at the Antiproton Decelerator (AD) at CERN. We performed a laser-microwave-laser resonance spectroscopy using a continuous wave (cw) pulse-amplified laser system and microwave cavity to measure the HF transition frequencies. Improvements in the spectral linewidth and stability of our laser system have increased the precision of these measurements by a factor of five and reduced the line width by a factor of three compared to our previous results. A compariso…
We report on the first experimental results for microwave spectroscopy of the hyperfine structure of antiprotonic He-3. Due to the helium nuclear spin, antiprotonic He-3 has a more complex hyperfine structure than antiprotonic He-4 which has already been studied before. Thus a comparison between theoretical calculations and the experimental results will provide a more stringent test of the three-body quantum electrodynamics (QED) theory. Two out of four super-super-hyperfine (SSHF) transition lines of the (n,L)=(36,34) state were observed. The measured frequencies of the individual transitions…
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…
The effect of microwave radiation on the resonance fluorescence of a cloud of cold $^{85}Rb$ atoms in a magnetooptical trap is studied. The radiation frequency was tuned near the hyperfine splitting frequency of rubidium atoms in the 5S ground state. The microwave field induced magnetic dipole transitions between the magnetic sublevels of the 5S(F=2) and 5S(F=3) states, resulting in a change in the fluorescence signal. The resonance fluorescence spectra were recorded by tuning the microwave radiation frequency. The observed spectra were found to be substantially dependent on the transition und…
We perform precision microwave spectroscopy--aided by Stark deceleration--to reveal the low magnetic field behavior of OH in its ^2Π_{3/2} ro-vibronic ground state, identifying two field-insensitive hyperfine transitions suitable as qubits and determining a differential Lande g-factor of 1.267(5)\times10^{-3} between opposite parity components of the Λ-doublet. The data are successfully modeled with an effective hyperfine Zeeman Hamiltonian, which we use to make a tenfold improvement of the magnetically sensitive, astrophysically important ΔF=\pm1 satellite-line frequencies, yielding 172052988…
The coupling between microwave fields and atoms (or atom-like systems) is inherently weaker than for optical fields, making microwave signal manipulation for applications like quantum information processing technically challenging. In order to better understand this coupling and to develop tools for measuring it, we explore the microwave coupling to atoms using the "atomic candle" technique, and push it beyond the bounds of the small-signal regime in order to deliver a larger signal. In familiar two-level systems, responses beyond the usual Rabi oscillations can arise when a single-tone drive …
Rare-earth ion doped crystals are promising systems for quantum communication and quantum information processing. In particular, paramagnetic rare-earth centres can be utilized to realize quantum coherent interfaces simultaneously for optical and microwave photons. In this article, we study hyperfine and magnetic properties of a Y$_2$SiO$_5$ crystal doped with $^{171}$Yb$^{3+}$ ions. This isotope is particularly interesting since it is the only rare--earth ion having electronic spin $S=\frac{1}{2}$ and nuclear spin $I=\frac{1}{2}$, which results in the simplest possible hyperfine level structu…
This work presents accurate ab initio determination of the hyperfine splitting for the ground state and few low-lying excited states of 113Cd+; important candidates for the frequency standard in the microwave region, using coupled-cluster theory (CC) in the relativistic framework. The calculated hyperfine splitting are well in agreement with recent experimental results. We have also carried out the lifetimes of the 5p2P1=2 and 5p2P3=2 states, which are in well agreement with recent experimental result (Moehring et al., PRA 73 023413, 2006). The roles of different electron correlation effects i…
We study the hyperfine spectrum of atoms of $^{87}$Rb dressed by a radio-frequency field, and present experimental results in three different situations: freely falling atoms, atoms trapped in an optical dipole trap and atoms in an adiabatic radio-frequency dressed shell trap. In all cases, we observe several resonant side bands spaced (in frequency) at intervals equal to the dressing frequency, corresponding to transitions enabled by the dressing field. We theoretically explain the main features of the microwave spectrum, using a semi-classical model in the low field limit and the Rotating Wa…
We study the ability to control d-dimensional quantum systems (qudits) encoded in the hyperfine spin of alkali-metal atoms through the application of radio- and microwave-frequency magnetic fields in the presence of inhomogeneities in amplitude and detuning. Such a capability is essential to the design of robust pulses that mitigate the effects of experimental uncertainty and also for application to tomographic addressing of particular members of an extended ensemble. We study the problem of preparing an arbitrary state in the Hilbert space from an initial fiducial state. We prove that inhomog…
We explore coherent multi-photon processes in $^{87}$Rb$^{133}$Cs molecules using 3-level lambda and ladder configurations of rotational and hyperfine states, and discuss their relevance to future applications in quantum computation and quantum simulation. In the lambda configuration, we demonstrate the driving of population between two hyperfine levels of the rotational ground state via a two-photon Raman transition. Such pairs of states may be used in the future as a quantum memory, and we measure a Ramsey coherence time for a superposition of these states of 58(9) ms. In the ladder configur…
Spectroscopy of the Hyperfine Structure of HD$^+$ in Rotationally Excited States with 10-ppb Uncertainty
ASML；Laboratoire Kastler Brossel, Sorbonne Université, CNRS, ENS-PSL Research University, Collège de France（卡斯勒-布罗塞尔实验室，索邦大学，法国国家科学研究中心，巴黎文理研究大学，法兰西学院）；LaserLaB, Department of Physics and Astronomy, Vrije Universiteit Amsterdam（激光实验室，阿姆斯特丹自由大学物理与天文系）；Science Institute and Faculty of Physical Sciences, University of Iceland（冰岛大学理学院和物理科学学院）
Individual-qubit addressing is a prerequisite for many instances of quantum information processing. We demonstrate this capability on trapped-ion qubits with microwave near-fields delivered by electrode structures integrated into a microfabricated surface-electrode trap. We describe four approaches that may be used in quantum information experiments with hyperfine levels as qubits. We implement individual control on two 25Mg+ ions separated by 4.3 micrometer and find spin-flip crosstalk errors on the order of 10^(-3).
Ultracold molecules offer entirely new possibilities for the control of quantum processes due to their rich internal structure. Recently, near quantum degenerate gases of molecules have been prepared in their rovibronic ground state. For future experiments, it is crucial to also control their hyperfine state. Here, we report the preparation of a rovibronic ground state molecular quantum gas in a single hyperfine state and in particular in the absolute lowest quantum state. The demonstrated and presented scheme is general for bialkali polar molecules and allows the preparation of molecules in a…
We perform spectroscopy on the hyperfine splitting of $^{85}$Rb atoms trapped in far-off-resonance optical traps. The existence of a spatially dependent shift in the energy levels is shown to induce an inherent dephasing effect, which causes a broadening of the spectroscopic line and hence an inhomogeneous loss of atomic coherence at a much faster rate than the homogeneous one caused by spontaneous photon scattering. We present here a number of approaches for reducing this inhomogeneous broadening, based on trap geometry, additional laser fields, and novel microwave pulse sequences. We then sh…
A dynamic blue-detuned optical dipole trap with stable $^{87}Rb$ atoms produces a differential ac Stark shift of 18 Hz in the ground state hyperfine transition, and it preserves the ground state hyperfine superpositions for a long coherence time of 180 ms. The trapped atoms undergoing microwave Rabi oscillations are sensitive to a small signal, artificially generated with a second microwave source, phase locked to the first allow- ing a simple and effective method for determining signal-to-noise ratio limits through interference techniques. This provides an excellent means of calibrating sensi…
Solid-state electronic spins are extensively studied in quantum information science, as their large magnetic moments offer fast operations for computing and communication, and high sensitivity for sensing. However, electronic spins are more sensitive to magnetic noise, but engineering of their spectroscopic properties, e.g. using clock transitions and isotopic engineering, can yield remarkable spin coherence times, as for electronic spins in GaAs, donors in silicon and vacancy centres in diamond. Here we demonstrate simultaneously induced clock transitions for both microwave and optical domain…
In this paper we report the development of the design verification model (DVM) of Rb atomic frequency standard. The Rb atomic frequency standard or clock has two distinct parts. One is the Physics Package where the hyperfine transitions produce the clock signal in the integrated filter cell configuration and the other is the electronic circuits which generate the resonant microwave hyperfine frequency, phase modulator and phase sensitive detector. In this paper the details of the Rb Physics package and the electronic circuits are given. The effect of putting the photo detector inside the micro…
Collisions of metastable antiprotonic helium atoms with atoms of the medium induce, among other processes, transitions between hyperfine structure (HFS) states, as well as shifts and broadening of microwave M1 spectral lines. In order to obtain matrix potential of interaction between $(\mathrm{\bar{p} He} ^+)$ and $\mathrm{He}$, we have calculated the potential energy surface (PES) in the framework of unrestricted Hartree-Fock method taking into account electron correlations in the second-order perturbation theory (MP2). With this potential, the system of close-coupling equations for HFS chann…
We demonstrate the cancellation of the differential ac Stark shift of the microwave hyperfine clock transition in trapped $^{87}$Rb atoms. Recent progress in metrology exploits so-called "magic wavelengths," whereby an atomic ensemble can be trapped with laser light whose wavelength is chosen so that both levels of an optical atomic transition experience identical ac Stark shifts. Similar magic-wavelength techniques are not possible for the microwave hyperfine transitions in the alkalis, due to their simple electronic structure. We show, however, that ac Stark shift cancellation is indeed achi…
We report a study of high-resolution microwave spectroscopy of nitrogen-vacancy centers in diamond crystals at and around zero magnetic field. We observe characteristic splitting and transition imbalance of the hyperfine transitions, which originate from level anti-crossings in the presence of a transverse effective field. We use pulsed electron spin resonance spectroscopy to measure the zero-field spectral features of single nitrogen-vacancy centers for clearly resolving such level anti-crossings. To quantitatively analyze the magnetic resonance behavior of the hyperfine spin transitions in t…
We report a technique that uses clouds of ultracold atoms as sensitive, tunable, and non-invasive probes for microwave field imaging with micrometer spatial resolution. The microwave magnetic field components drive Rabi oscillations on atomic hyperfine transitions whose frequency can be tuned with a static magnetic field. Readout is accomplished using state-selective absorption imaging. Quantitative data extraction is simple and it is possible to reconstruct the distribution of microwave magnetic field amplitudes and phases. While we demonstrate 2d imaging, an extension to 3d imaging is straig…
Atomic magnetometry is one of the most sensitive ways to measure magnetic fields. We present a method for converting a naturally scalar atomic magnetometer into a vector magnetometer by exploiting the polarization dependence of hyperfine transitions in rubidium atoms. First, we fully determine the polarization ellipse of an applied microwave field using a self-calibrating method, i.e. a method in which the light-atom interaction provides everything required to know the field in an orthogonal laboratory frame. We then measure the direction of an applied static field using the polarization ellip…
