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 contamination from the second-order corrections. Measurements to the required accuracy should be possible with a single trapped barium ion using sensitive techniques already demonstrated in Ba$^+$ experiments.
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…
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…
We present precision measurements of the hyperfine intervals in the 5D3/2 manifold of a single trapped Barium ion, 137 Ba+ . Measurements of the hyperfine intervals are made between mF = 0 sublevels over a range of magnetic fields allowing us to interpolate to the zero field values with an accuracy below a few Hz, an improvement on previous measurements by three orders of magnitude. Our results, in conjunction with theoretical calculations, provide a 30-fold reduction in the uncertainty of the magnetic dipole (A) and electric quadrupole (B) hyperfine constants. In addition, we obtain the magne…
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, $^{25}…
Hyperfine-structure constants of odd Ra$^{+}$ 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 $…
We measure hyperfine structure in the metastable ${^3P}_2$ state of $^{173}$Yb and extract the nuclear magnetic octupole moment. We populate the state using dipole-allowed transitions through the ${^3P}_1$ and ${^3S}_1$ states. We measure frequencies of hyperfine transitions of the ${^3P}_2 \rightarrow {^3S}_1$ line at 770 nm using a Rb-stabilized ring cavity resonator with a precision of 200 kHz. Second-order corrections due to perturbations from the nearby ${^3P}_1$ and ${^1P}_1$ states are below 30 kHz. We obtain the hyperfine coefficients as: $A=-742.11(2)$ MHz, $B=1339.2(2)$ MHz, which re…
We perform precision measurements on the 5D$_{5/2}$ manifold hyperfine intervals of a single trapped ion, $^{137}$Ba$^+$. RF spectroscopy is used to measure the hyperfine intervals to an accuracy of a few Hz. Our results provide a three orders of magnitude improvement in accuracy over previous work and also provide a 10-fold improvement in the value of $g_J$ for this level. These results complement our previous work on the 5D$_{3/2}$ manifold of $^{137}$Ba$^+$, providing an independent measurement of the nuclear octupole, and a consistency check on atomic structure calculations.
Hyperfine structures of $^{211}$Fr due to the interactions of magnetic dipole ($μ$), electric quadrupole ($Q$) and magnetic octupole ($Ω$) moments with the electrons are investigated using the relativistic coupled-cluster (RCC) theory with an approximation of singles, doubles and important valence triples excitations in the perturbative approach. Validity of our calculations are substantiated by comparing the results with their available experimental values. Its $Q$ value has also been elevated by combining the measured hyperfine structure constant of the $7p \ ^2P_{3/2}$ state with our improv…
Hyperfine structure (HFS) of atomic energy levels arises due to interactions of atomic electrons with a hierarchy of nuclear multipole moments, including magnetic dipole, electric quadrupole and higher rank moments. Recently, a determination of the magnetic octupole moment of the $^{173}\mathrm{Yb}$ nucleus was reported from HFS measurements in neutral ${}^{173}\mathrm{Yb}$ [PRA 87, 012512 (2013)], and is four orders of magnitude larger than the nuclear theory prediction. Considering this substantial discrepancy between the spectroscopically extracted value and nuclear theory, here we propose …
The hyperfine constants of the $^3$P$^{\circ}_2$ state in neutral Yb have been measured using three different dipole transitions. This state was recently shown to have a comparatively large hyperfine magnetic octupole splitting, and thus a puzzlingly large magnetic octupole moment. The measurement is performed using collinear laser spectroscopy on a fast atomic beam, which provides a straightforward route to probing long-lived metastable atomic states with high resolution. From the combined analysis of all three lines we find no significant evidence for a non-zero octupole moment in $^{173}$Yb…
We report the measurement of the hyperfine splitting in the $7D_{5/2}$ state of $^{133}$Cs using high resolution Doppler-free two-photon spectroscopy enabled by precise frequency scans using an acousto-optic modulator. All the six hyperfine levels are resolved in our spectra. We determine the hyperfine coupling constants A = -1.70867(62) MHz and B = 0.050(14) MHz which represent over 20-times improvement in the precision of both A and B. Moreover, our measurement is sufficiently precise to put bounds on the value of the magnetic octupole coupling constant C = 0.4(1.4) kHz for the $7D_{5/2}$ st…
The existence of a nuclear electric octupole moment (EOM) requires both parity and time invariance violation. The EOMs of odd $Z$ nuclei that are induced by a particular T- and P-odd interaction are calculated. We compare such octupole moments with the collective EOMs that can occur in nuclei having a static octupole deformation. A nuclear EOM can induce a parity and time invariance violating atomic electric dipole moment, and the magnitude of this effect is calculated. The contribution of a nuclear EOM to such a dipole moment is found, in most cases, to be smaller than that of other mechanism…
$^{229}$Th is a promising candidate for developing a nuclear optical clock and searching the new physics beyond the standard model. Accurate knowledge of the nuclear properties of $^{229}$Th is very important. In this work, we calculate hyperfine-structure constants for the first four states of $^{229}$Th$^{3+}$ using the relativistic coupled-cluster method based on the Gauss basis set. The no-pair Dirac-Coulomb-Breit Hamiltonian with the lowest-order quantum electrodynamics (QED) correction is the starting point, together with all linear and non-linear terms of single and double excitations a…
Parity (P) and time reversal (T) violating nuclear forces create P, T -odd moments in expansion of the nuclear electrostatic potential. We derive expression for the nuclear electric octupole field which includes the electron screening correction (similar to the screening term in the Schiff moment). Then we calculate the Z alpha corrections to the Schiff moment which appear due to the finite nuclear size. Such corrections are important in heavy atoms with nuclear charge Z > 50. The Schiff and octupole moments induce atomic electric dipole moments (EDM) and P, T -odd interactions in molecules wh…
Parity and time invariance violating (${\cal P},{\cal T}$-odd) nuclear forces produce ${\cal P},{\cal T}$-odd nuclear moments, for example, the nuclear Schiff moment. In turn, this moment can induce electric dipole moments (EDMs) in atoms. We estimate the contribution to the Schiff moment from the soft collective octupole vibrations existing in many heavy nuclei. Two possible mechanisms are considered, mixing of the ground state of an odd-$A$ nucleus with the octupole phonon state, and ${\cal P},{\cal T}$-odd admixture to the single-particle wave function of the valence nucleon. We found pract…
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…
Nuclear forces violating parity and time reversal invariance P,T-odd produce P,T-odd nuclear moments, for example, the nuclear Schiff moment. In turn, this moment can induce the electric dipole moment (EDM) in the atom. The contribution to the Schiff moment from the soft collective quadrupole and octupole vibrations in spherical nuclei is calculated in the framework of the quasiparticle random phase approximation with separable quadrupole and octupole forces. The values of nuclear Schiff moments predicted for odd 217-221Ra and 217-221Ra isotopes indicate a possibility of enhancement by a facto…
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 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 …
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…
Nuclei with an octupole deformation have a non-zero electric octupole moment, electric dipole moment (EDM), Schiff moment and magnetic quadrupole moment (MQM) in the intrinsic frame which rotates with the nucleus. In a state with definite angular momentum in the laboratory frame, these moments are forbidden by parity (P) and time reversal invariance (T) conservation, meaning their expectation values vanish due to nuclear rotation. However, nuclei with an octupole deformation have doublets of close opposite parity rotational states with the same spin, which are mixed by T,P-odd nuclear forces. …
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+)…
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…
Nuclei with static intrinsic octupole deformation or a soft octupole vibrational mode lead to strongly enhanced collective nuclear Schiff? moments. Interaction between electrons and these Schiff moments produce enhanced time reversal (T) and parity (P) violating electric dipole moments (EDM) in atoms and molecules. Corresponding experiments may be used to test CP-violation theories predicting T,P-violating nuclear forces and to search for axions. Nuclear octupole deformations are predicted in many short lived isotopes. This paper investigates octupole deformations in stable and very long lifet…
We perform high resolution spectroscopy on $^{176}$Lu$^+$ including the $^1S_0\leftrightarrow{^3}D_1$ and $^1S_0\leftrightarrow{^3}D_2$ clock transitions. Hyperfine structures and optical frequencies relative to the $^1S_0$ ground state of four low lying excited states are given to a few tens of kHz resolution. This covers the most relevant transitions involved in clock operation with this isotope. Additionally, measurements of the $^3D_2$ hyperfine structure may provide access to higher order nuclear moments, specifically the magnetic octupole and electric hexadecapole moments.
We use relativistic Hartree-Fock and correlation potential methods to calculate nuclear spin-dependent parity non-conserving amplitudes (dominated by the nuclear anapole moment) between hyperfine structure components of the ground state of odd isotopes of K, Rb, Cs, Ba+, Yb+, Tl, Fr, and Ra+. The results are to be used for interpretation of current and future measurements.
Accurate calculations of the fine and hyperfine splitting of the 2P state in Li and Be$^+$ isotopes using the explicitly correlated Hylleraas basis set are presented. Theoretical predictions including the mixing of $P_{1/2}$ and $P_{3/2}$ states, relativistic and quantum electrodynamics effects on hyperfine interactions, are compared with experimental values. It is concluded that precise spectroscopic determination of the nuclear magnetic moments requires elimination of nuclear structure effects by combining measurements for two different states.
The hyperfine splitting of the ground state of H-, Li-, and B-like ions is investigated in details within the range of nuclear numbers Z = 7-28. The rigorous QED approach together with the large-scale configuration-interaction Dirac-Fock-Sturm method are employed for the evaluation of the interelectronic-interaction contributions of first and higher orders in 1/Z. The screened QED corrections are evaluated to all orders in (αZ) utilizing an effective potential approach. The influence of nuclear magnetization distribution is taken into account within the single-particle nuclear model. The speci…
Sturmian basis set for the Dirac equation with finite nuclear size: Application to polarizability, Zeeman and hyperfine splitting, and vacuum polarization
The hyperfine anomalies in Gd and Nd have been extracted from the experimental hyperfine structure constants using a new method. In addition to the values of the hyperfine anomaly new improved values of the nuclear magnetic dipole moment ratios are derived.
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.
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 …
High precision spectroscopy of the $^1S_0$-to-${^1}D_2$ clock transition of $^{176}$Lu is reported. Measurements are performed with Hertz level precision with the accuracy of the hyperfine-averaged frequency limited by the calibration of an active hydrogen maser to the SI definition of the second via a GPS link. The measurements also provide accurate determination of the $^1D_2$ hyperfine structure. Hyperfine structure constants associated with the magnetic octupole and electric hexadecapole moments of the nucleus are considered, which includes a derivation of correction terms from third-order…
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.
Relativistic and QED corrections were calculated for hyperfine splitting of the $2S_{1/2}$ ground state in $^{6,7}$Li atoms with an exact account for electronic correlations. The resulting theoretical predictions achieved such a precision level that, by comparison with experimental values, they enable determination of the nuclear properties. In particular, the obtained results show that the $^7$Li nucleus, having a charge radius smaller than $^6$Li, has about a 40% larger Zemach radius. Together with known differences in the electric quadrupole and magnetic dipole moments, this calls for a dee…
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 report a fourfold improvement in the determination of nuclear magnetic moments for neutron-deficient isotopes of francium-207--213, reducing the uncertainties from 2% for most isotopes to 0.5%. These are found by comparing our high-precision calculations of hyperfine structure constants for the ground states with experimental values. In particular, we show the importance of a careful modeling of the Bohr-Weisskopf effect, which arises due to the finite nuclear magnetization distribution. This effect is particularly large in Fr and until now has not been modeled with sufficiently high accura…
A recent measurement of the hyperfine splitting in the ground state of Li-like $^{209}$Bi$^{80+}$ has established a "hyperfine puzzle" -- the experimental result exhibits a 7$σ$ deviation from the theoretical prediction [J. Ullmann et al., Nat. Commun. 8, 15484 (2017); J. P. Karr, Nat. Phys. 13, 533 (2017)]. We provide evidence that the discrepancy is caused by an inaccurate value of the tabulated nuclear magnetic moment ($μ_I$) of $^{209}$Bi. We perform relativistic density functional theory and relativistic coupled cluster calculations of the shielding constant that should be used to extract…
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.
