We have performed accurate calculations of the hyperfine structure of the $2\,^3\!P$ state in the $^9$Be atom with the help of highly optimized, explicitly correlated functions, accounting for the leading finite nuclear mass, radiative, nuclear structure and relativistic effects. By comparison with measurements, we have determined the $^9$Be nuclear quadrupole moment to be $Q_{\rm N} = 0.05350(14)$ barns, which is not only the most accurate result, but also disagrees with previous determinations.
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 report the magnetic dipole and electric quadrupole hyperfine coupling constants of 6 P_{3/2} state of ^{133} Cs(I= {7/2}) obtained from the relativistic coupled cluster (RCC) method. To our knowledge, no prior electric quadrupole hyperfine CC calculation is available for ^{133} Cs(6 P_{3/2}) state. Our computed magnetic dipole (A) and electric quadrupole (B) coupling constants are in excellent agreement with the experiment.
The quantum resonances of an atom possessing a single valence electron which shows hyperfine interaction with the nucleus is investigated in the presence of a three dimensional magnetic quadrupole field. Particular emphasis is put on the study of the interplay of the hyperfine and quadrupole forces. Analyzing the underlying Hamiltonian a variety of symmetries are revealed which give rise to a two-fold degeneracy of the resonance energies. Our numerical approach employs the complex scaling method and a Sturmian basis set. Several regimes and classes of short-lived and long-lived resonances are …
We evaluate the electric quadrupole moments of the ${^1}\!S_0$ and ${^3}\!P_0$ clock states of $^{27}$Al$^+$ and $^{115}$In$^+$. To capture all dominant contributions, our analysis extends through third order of perturbation theory and includes hyperfine coupling of the electrons to both the magnetic dipole and electric quadrupole moments of the nucleus. For $^{27}$Al$^+$, a fortuitous cancellation leads to a suppressed frequency shift. This should allow for continued improvement of the clock without special techniques to control or cancel the shift, such as the averaging schemes that are crit…
The relativistic multiconfiguration Dirac-Hartree-Fock (MCDHF) and the non-relativistic multiconfiguration Hartree-Fock (MCHF) methods have been employed to calculate the magnetic dipole and electric quadrupole hyperfine structure constants of zinc. The calculated electric field gradients for the $ 4s 4p \,\, ^3 \! P^o_{1} $ and $ 4s 4p \,\, ^3 \! P^o_{2} $ states, together with experimental values of the electric quadrupole hyperfine structure constants, made it possible to extract a nuclear electric quadrupole moment $ Q(^{67}{\rm Zn}) = 0.122(10) $ b. The error bar has been evaluated in a q…
Hyperfine-induced electric dipole contributions may significantly increase probabilities of otherwise very weak electric octupole and magnetic quadrupole atomic clock transitions (e.g. transitions between $s$ and $f$ electron orbitals). These transitions can be used for exceptionally accurate atomic clocks, quantum information processing and search for dark matter. They are very sensitive to new physics beyond the Standard Model, such as temporal variation of the fine structure constant, the Lorentz invariance and Einstein equivalence principle violation. We formulate conditions under which th…
By combining our theoretical calculation and recently measured electric quadrupole hyperfine structure constant of the $3d ^2D_{5/2}$ state in the singly ionized $^{43}$Ca, we determine its nuclear quadrupole moment to one percent accuracy. The obtained result, $-0.0444(6)b$, is about ten percent improvement over the considered standard value. We have employed the relativistic coupled-cluster theory at single and double excitations level to calculate the electronic wave functions. The accuracy of these wave functions are estimated by comparing our calculated magnetic dipole hyperfine constants…
We have employed the relativistic coupled cluster theory to calculate the magnetic dipole and electric quadrupole hyperfine constants for the ground and low lying excited states of singly ionized magnesium. Comparison with experimental and the other theoretical results are done and predictions are also made for a few low lying excited states which could be of interest. We have made comparative studies of the important many body effects contributing to the hyperfine constants for the different states of the ion.
We report results of a theoretical investigation of hyperfine interactions in two homonuclear isotopologues of the hydrogen molecule: H$_{2}$ and D$_{2}$. We present a set of hyperfine coupling constants: spin-rotation, spin-spin dipole and, in the case of the D$_{2}$ molecule, electric quadrupole coupling constants for all bound states of the two isotopologues in their ground electronic $X^{1}Σ^{+}_{g}$ state. We provide a list of positions and intensities of 220 997 hyperfine components of 16 079 rovibrational quadrupole transitions of the O, Q and S branches. The positions and intensities o…
Atomic quadrupole moments and hyperfine constants of the metastable $^2 D_{3/2, 5/2}$ states of Ca$^+$, Sr$^+$, Ba$^+$, Yb$^+$, and Hg$^+$ are calculated by the multiconfiguration Dirac-Hartree-Fock and relativistic configuration-interaction methods. For Hg$^+$, the configuration is $5d^9 6s^2$. For the other ions, the configuration consists of a single $d$-electron outside a set of closed shells. Current interest in the quadrupole moments of these states is due to the fact that optical transitions of these ions may be useful as references for frequency standards. Energy shifts of the metastab…
We investigate electric quadrupole hyperfine structure constant ($B$) results in $^{135}$Ba$^+$ and $^{137}$Ba$^+$ and compare their ratios with the reported measurements of the ratio between the nuclear quadrupole moment ($Q$) values of these isotopes. We carry out confidence tests for the reported experimental $B$ values and calculations of $B/Q$ from the present work. Inconsistencies in the experimental $B$ values are observed in both the isotopes from different experiments performed using the same techniques. The present calculations are carried out using an all order relativistic many-bod…
Molecular hydrogen ions are of metrological relevance due to the possibility of precise theoretical evaluation of their spectrum and of external-field-induced shifts. In homonuclear molecular ions the electric dipole $E1$ transitions are strongly suppressed, and of primary laser spectroscopy interest is the electric quadrupole ($E2$) transition spectrum. In continuation of previous work on the H$_2^+$ ion, we report here the results of the calculations of the hyperfine structure of the laser-induced electric quadrupole transitions between a large set of ro-vibrational states of D$_2^+$; the in…
Large scale ab initio calculations of the electric contribution (i.e. the electric field gradient) to the electric quadrupole hyperfine interaction constants $B$ for the $5p~^2P_{3/2}$ state in $^{109}$Cd$^+$ ion and the $5s5p~^3P_{1,2}$ states in neutral $^{109}$Cd atom were performed. To probe the sensitivity of $B$ to different electron correlation effects, six sets of variational multi-configuration Dirac-Hartree-Fock and relativistic configuration interaction calculations employing different strategies were carried out. The calculated electric field gradients, together with experimental v…
Hyperfine-structure constants of odd Ra$^{+}$ due to the interactions of nuclear magnetic dipole, electric quadrupole, and magnetic octupole moments with the electrons are investigated in the framework of relativistic coupled-cluster method within single- and double-excitation approximation. The calculated energies and magnetic dipole hyperfine-structure constants $A$ exhibit a good agreement with available experimental values. Combining with the experimental electric quadrupole hyperfine-structure constant, we also extracted the electric quadrupole moments $Q$ of $^{209,211,221,223}$Ra. Our $…
The values of nuclear electric quadrupole moment are different by about 7% for 87Sr nucleus between the recommended value [N. J. Stone, At. Data Nucl. Data Tables 111-112, 1 (2016); P. Pyykko, Mol. Phys. 116, 1328 (2018)] and earlier results [e.g. A. M. Matensson-Pendrill, J. Phys. B: At. Mol. Opt. Phys. 35, 917 (2002); K. Z. Yu et al., Phys. Rev. A 70, 012506 (2004)]. In this work, we reported a new value, Q(87Sr) = 328(4) mb, making use of our calculated electric field gradients produced by electrons at nucleus in combination with experimental values for hyperfine structures of the 5s5p 3P1,…
Relativistic formulas for the electric quadrupole moment of a hydrogenlike atom, induced by the hyperfine interaction, are derived for $ns_{1/2}$ and $np_{1/2}$ states. Both the magnetic dipole and electric quadrupole hyperfine interactions are taken into account. The formulas are valid for ions with arbitrary nuclear charge and spin. The induced quadrupole moment is compared with the nuclear quadrupole moment for a wide range of hydrogenlike ions.
Searching for an accurate optical clock which can serve as a better time standard than the present day atomic clock is highly demanding from several areas of science and technology. Several attempts have been made to built more accurate clocks with different ion species. In this article we discuss the electric quadrupole and hyperfine shifts in the $5d^{9}6s^{2} ^{2}D_{5/2}(F=0,m_{F}=0)\leftrightarrow5d^{10}6s ^{2}S_{1/2}(F=2,m_{F}=0)$ clock transition in $ ^{199}Hg^{+}$, one of the most promising candidates for next generation optical clocks. We have applied Fock-space unitary coupled-cluster…
A method for precise calculation of the energy corrections due to second order electric quadrupole interactions, as well as mixed electric quadrupole-vacuum polarization in the framework of the dynamic hyperfine structure in heavy muonic atoms is presented. For this, a multipole expansion of the Uehling potential is performed. The approach is applicable for an arbitrary nuclear electric charge distribution. By performing these calculations for muonic Rhenium and Uranium using a deformed Fermi distribution, it is shown that both corrections contribute on a level presumably visible in upcoming e…
We consider hyperfine-mediated effects for clock transitions in $^{176}$Lu$^+$. Mixing of fine structure levels due to the hyperfine interaction bring about modifications to Landé $g$-factors and the quadrupole moment for a given state. Explicit expressions are derived for both $g$-factor and quadrupole corrections, for which leading order terms arise from the nuclear magnetic dipole coupling. High accuracy measurements of the $g$-factors for the $^1S_0$ and $^3D_1$ hyperfine levels are carried out, which provide an experimental determination of the leading order correction terms.
We investigate the hyperfine energy levels and Zeeman splittings for homonuclear alkali-metal dimers in low-lying rotational and vibrational states, which are important for experiments designed to produce quantum gases of deeply bound molecules. We carry out density-functional theory (DFT) calculations of the nuclear hyperfine coupling constants. For nonrotating states, the zero-field splittings are determined almost entirely by the scalar nuclear spin-spin coupling constant. By contrast with the heteronuclear case, the total nuclear spin remains a good quantum number in a magnetic field. We a…
The multiconfiguration Dirac-Hartree-Fock (MCDHF) model has been employed to calculate the expectation values for the hyperfine splittings of the 5d96s2 2D3/2 and 5d96s2 2D5/2 levels of atomic gold. One-, two-, and three-body electron correlation effects involving all 79 electrons have been included in a systematic manner. The approximation employed in this study is equivalent to a Complete Active Space (CAS) approach. Calculated electric field gradients, together with experimental values of the electric quadrupole hyperfine structure constants, allow us to extract a nuclear electric quadrupol…
The hyperfine structures of the $2\,^3\!S_1$ and $2\,^3\!P_J$ states of the $^7$Be$^{2+}$ and $^9$Be$^{2+}$ ions are investigated within the framework of the nonrelativistic quantum electrodynamics (NRQED). The uncertainties of present hyperfine splitting results of $^9$Be$^{2+}$ are in the order of several tens of ppm, where two orders of magnitude improvement over the previous theory and experiment values has been achieved. The contribution of nuclear electric quadrupole moment to hyperfine splitting of $^7$Be$^{2+}$ has been studied. A scheme for determining the properties of Be nuclei in t…
Determination of nuclear moments for many nuclei relies on the computation of hyperfine constants, with theoretical uncertainties directly affecting the resulting uncertainties of the nuclear moments. In this work we improve the precision of such method by including for the first time an iterative solution of equations for the core triple cluster amplitudes into the relativistic coupled-cluster method, with large-scale complete basis sets. We carried out calculations of the energies and magnetic dipole and electric quadrupole hyperfine structure constants for the low-lying states of 229Th^(3+)…
We show that by averaging over transitions to multiple hyperfine levels, quadrupole shifts and dominant Zeeman effects exactly cancel whenever the nuclear spin, I, is at least as large as the total electronic angular momentum, J. The average frequency thus defines a frequency reference which is inherently independent of external magnetic fields and electric field gradients. We use Lu+ to illustrate the method although the approach could be readily adapted to other atomic species. This approach practically eliminates the quadrupole and Zeeman shift considerations for many clock candidates.
We calculate the A and B hyperfine constants for the low-lying states of 229Th3+ using a high-precision relativistic all-order approach. By combining these calculations with measurements of the 6d and 5f hyperfine constants [C. J. Campbell et al., Phys. Rev. Lett. 106, 223001 (2011)], we determine the magnetic dipole μ=0.360(7)μ_B and the electric-quadrupole Q=3.11(6) eb moments of the 229Th nucleus. Our value for μis five times more accurate and is 22% smaller than the best previous value μ=0.46(4) μ_B [S. Gerstenkorn et al., J. Phys. (Paris) 35, 483 (1974)], while our value for Q is the same…
We have investigated the correction to the hyperfine structure of heavy multicharged ions, which is connected with the nuclear-polarization effect caused by the unpaired bound electron. Numerical calculations are performed for hydrogenlike ions taking into account the dominant collective nuclear excitations. The correction defines the ultimate limit of precision in accurate theoretical predictions of the hyperfine-structure splittings.
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…
Energy levels, magnetic dipole, and electric quadrupole hyperfine structure of the superheavy element rutherfordium (Rf, $Z$=104) and its first three ions are calculated using a combination of the configuration interaction, coupled-cluster single-doubles, and many-body perturbation theory techniques. The results are to be used in future interpretations of the measurements in terms of nuclear magnetic dipole and electric quadrupole momenta. To have a guide on the accuracy of the study, we perform similar calculations for hafnium (Hf, $Z$=72) and its ions. Hf is a lighter analog of Rf with a sim…
Calculations of the magnetic hyperfine structure rely on the input of nuclear properties -- nuclear magnetic moments and nuclear magnetization distributions -- as well as quantum electrodynamic (QED) radiative corrections for high-accuracy evaluation in heavy atoms. The uncertainties associated with assumed values of these properties limit the accuracy of hyperfine calculations. For example, for the heavy alkali-metal atoms Cs and Fr, these uncertainties may amount collectively to almost 1\% or 2\%, respectively. In this paper we propose a method for removing the dependence of hyperfine struct…
The hyperfine splitting in hydrogenlike $^{209}$Bi, $^{203}$Tl, and $^{205}$Tl is calculated with the nuclear magnetization determined from experimental data on the hyperfine splitting in the corresponding muonic atoms. The single-particle and configuration-mixing nuclear models are considered. The QED corrections are taken into account for both electronic and muonic atoms. The obtained results are compared with other calculations and with experiment.
The magnetic octupole moment of 87Rb is determined from hyperfine intervals in the 5p 2P[3/2] state measured by Ye et al. [Opt. Lett. 21, 1280 (1996)]. Hyperfine constants A = 84.7189(22) MHz, B = 12.4942(43) MHz, and C = -0.12(09) kHz are obtained from the published measurements. The existence of a significant value for C indicates the presence of a nuclear magnetic octupole moment Omega. Combining the hyperfine constants with atomic structure calculations, we obtain Omega = -0.58(39) (b muN). Second-order corrections arising from interaction with the nearby 5p 2P[1/2] state are found to be i…
A theoretical model of hyperfine spectra of nuclear spin conversion of molecular isomers has been developed. The model takes into account the nuclear spin-spin and spin-rotation interactions, as well as the saturation of intramolecular mixing of molecular ortho and para states. The model has been applied to hyperfine spectra of nuclear spin conversion in ^{13}CH3F molecules subjected to an external electric field. Conditions under which the hyperfine structure in the spectra can be resolved have been determined.
The interaction of orbital electrons with the charge and magnetic moment of the nucleus polarizes it, and the detailed description requires a careful treatment of the nuclear vector polarizability. We present a complete and closed form expression for the resulting contribution to hyperfine splitting in light atomic systems.
Nuclear structure corrections of orders $Zα\, E_F$ and $(Zα)^2 E_F$ are calculated for the hyperfine splitting of the muonic deuterium. The obtained results disagree with previous calculations and lead to a $5\,σ$ disagreement with the current experimental value of the $2S$ hyperfine splitting in $μ$D.
We demonstrate the importance of electron correlation effects in the hyperfine structure constants of many low-lying states in $^{210}$Fr and $^{212}$Fr. This is achieved by calculating the magnetic dipole and electric quadrupole hyperfine structure constants using the Dirac-Fock approximation, second order many-body perturbation theory and the coupled-cluster method in the singles and doubles approximation in the relativistic framework. By combining our recommended theoretical results with the corresponding experimental values, improved nuclear magnetic dipole and electric quadrupole moments …
A recently developed version of the configuration interaction (CI) method for open shells with a large number of valence electrons has been used to study two heavy atoms, californium (Cf, Z= 98) and einsteinium (Es, Z= 99). Motivated by experimental work to measure the hyperfine structure (HFS) for these atoms, we perform the calculations of the magnetic dipole HFS constants $A$ and electric quadrupole HFS constant $B$ for the sake of interpretation of the measurements in terms of nuclear magnetic moment $μ$ and electric quadrupole moment $Q$. For verification of our computations, we have also…
We report the value of the electric quadrupole moment of $^{209}$Bi extracted from the atomic data. For this, we performed electronic structure calculations for the ground $^4S^o_{3/2}$ and excited $^2P^o_{3/2}$ states of atomic Bi using the Dirac-Coulomb-Breit Hamiltonian and the Fock space coupled cluster method with single, double, and full triple amplitudes for the three-particle Fock space sector. The value of the quadrupole moment of $^{209}$Bi, $Q(^{209}$Bi$)=-418(6)$~mb, derived from the resulting electric field gradient values and available atomic hyperfine splittings is in excellent …
Narrow linewidth signals of Electromagnetically Induced Transparency (EIT) in the metastable 83Kr have been observed for the first time. Various hyperfine transitions in 4p55s[3/2]2 to 4p55p[5/2]3 manifolds of 83Kr have been identified through the experimentally observed EIT signals. Some unresolved or poorly resolved hyperfine transitions in saturated absorption spectroscopy (SAS) are clearly resolved in the present work. Using the spectral separation of these EIT identified hyperfine transitions, the magnetic hyperfine constant (A) and the electric quadrupole hyperfine constant (B) are deter…
Using 201Hg+ contained within a linear quadrupole rf ion trap that is part of an atomic clock, we report the first high-resolution spectroscopy on the hyperfine structure of 201Hg+. We measure the absolute ground state hyperfine interval to be 29.954365821130(171)(62)(10) GHz, more than 8 orders of magnitude improvement over the previous measurement. The first error estimate in parentheses is the statistical error in the shifted line center measurement, the second is systematic uncertainty, and the third is calibration uncertainty in the hydrogen maser reference standard. By comparison to the …
The hyperfine structure of the long-lived $5D_{3/2}$ and $5D_{5/2}$ levels of Ba$^+$ ion is analyzed. A procedure for extracting relatively unexplored nuclear magnetic moments $Ω$ is presented. The relevant electronic matrix elements are computed in the framework of the ab initio relativistic many-body perturbation theory. Both the first- and the second-order (in the hyperfine interaction) corrections to the energy levels are analyzed. It is shown that a simultaneous measurement of the hyperfine structure of the entire $5D_J$ fine-structure manifold allows one to extract $Ω$ without contaminat…
The ground state hyperfine splitting values of high Z hydrogenlike ions are calculated. The relativistic, nuclear and QED corrections are taken into account. The nuclear magnetization distribution correction (the Bohr-Weisskopf effect) is evaluated within the single particle model with the g_{S}-factor chosen to yield the observed nuclear moment. An additional contribution caused by the nuclear spin-orbit interaction is included in the calculation of the Bohr-Weisskopf effect. It is found that the theoretical value of the wavelength of the transition between the hyperfine splitting components …
Ab initio calculations have been carried out to study the magnetic dipole and electric quadrupole hyperfine structure constants of $^{205}$Pb$^+$. Many-body effects have been considered to all orders using the relativistic coupled-cluster theory in the singles, doubles and partial triples approximation. The trends of these effects are found to be different from atomic systems that have been studied earlier.
Large-scale $\textit{ab initio}$ calculations of the electric field gradient, which constitutes the electronic contribution to the electric quadrupole hyperfine constant $B$, were performed for the $5s^25p6s$ $^{1,3}\!P^{\rm o}_1$ excited states of tin, using three independent computational strategies of the variational multiconfiguration Dirac-Hartree-Fock method and a fourth approach based on the configuration interaction Dirac-Fock-Sturm theory. For the $5s^25p6s$ $^{1}\!P^{\rm o}_1$ state, the final value of $B/Q =703(50)$ MHz/b differs by $0.4\%$ from the one recently used by Yordanov ${\…
A large-scale relativistic configuration-interaction (CI) calculation is performed for the magnetic-dipole and the electric-quadrupole hyperfine structure splitting in ^{7,6}Li and ^9Be^+. Numerical results for the 2^2S, 3^2S, 2^2P_{1/2}, and 2^2P_{3/2} states are reported. The CI calculation based on the Dirac-Coulomb-Breit Hamiltonian is supplemented with separate treatments of the QED, nuclear-magnetization distribution, recoil, and negative-continuum effects.
To search for the temporal variation of the fundamental constants one needs to know dependence of atomic transition frequencies on these constants. We study the dependence of the hyperfine structure of atomic $s$-levels on nuclear radius and, via radius, on quark masses. An analytical formula has been derived and tested by the numerical relativistic Hartree-Fock calculations for Rb, Cd$^+$, Cs, Yb$^+$ and Hg$^+$. The results of this work allow the use of the results of past and future atomic clock experiments and quasar spectra measurements to put constrains on time variation of the quark mass…
We report on our calculations of differential hyperfine anomalies in the nuclear single-particle model for a number of atoms and ions of interest for studies of fundamental symmetries violations. Comparison with available experimental data allows one to discriminate between different nuclear magnetization models, and this data supports the use of the nuclear single-particle model over the commonly-used uniform ball model. Accurate modelling of the nuclear magnetization distribution is important for testing atomic theory through hyperfine comparisons. The magnetization distribution must be adeq…
Measuring the hyperfine structure (HFS) of long-lived $^3P_2$ states of divalent atoms may offer the opportunity of extracting relatively unexplored nuclear magnetic octupole and electric hexadecapole moments. Here, using relativistic many-body methods of atomic structure and the nuclear shell model, we evaluate the effect of these higher nuclear moments on the hyperfine structure. We find that the sensitivity of HFS interval measurements in $^{87}$Sr needed to reveal the perturbation caused by the nuclear octupole moment is on the order of kHz. Results of similar analyses for $^{9}$Be, $^{25}…
