Search

The population dynamics of the 229Th isomeric state is studied in a solid-state host under laser illumination. A photoquenching process is observed, where off-resonant vacuum-ultraviolet (VUV) radiation leads to relaxation of the isomeric state. The cross-section for this photoquenching process is measured and a model for the decay process, where photoexcitation of electronic states within the material bandgap opens an internal conversion decay channel, is presented and appears to reproduce the measured cross-section., Comment: 7 pages, 6 figures

Laser excitation of thorium-229 nuclei in doped wide bandgap crystals has been demonstrated recently, opening the possibility of developing ultrastable solid-state clocks and sensitive searches for new physics. We develop a quantitative theory of the internal conversion of isomeric thorium-229 in solid-state hosts. The internal conversion of the isomer proceeds by resonantly exciting a valence band electron to a defect state, accompanied by multi-phonon emission. We demonstrate that, if the process is energetically allowed, it generally quenches the isomer on timescales much faster than the isomer's radiative lifetime, despite thorium being in the +4 charge state in the valence band.

The recent laser excitation of the 229Th isomeric transition in a solid-state host opens the door for a portable solid-state nuclear optical clock. However, at present the vacuum-ultraviolet laser systems required for clock operation are not conducive to a fieldable form factor. Here, we propose a possible solution to this problem by using 229Th-doped nonlinear optical crystals, which would allow clock operation without a vacuum-ultraviolet laser system and without the need of maintaining the crystal under vacuum.

The self-consistent inclusion of plasma effects in opacity calculations is a significant modeling challenge. As density increases, such effects can no longer be treated perturbatively. Building on a recently published model that addresses this challenge, we calculate opacities of oxygen at solar interior conditions. The new model includes the effects of treating the free electrons consistently with the bound electrons, and the influence of free electron energy and entropy variations are explored. It is found that, relative to a state-of-the-art-model that does not include these effects, the bound free-opacity of the oxygen plasmas considered can increase by 10%.

After nearly fifty years of searching, the vacuum ultraviolet $^{229}$Th nuclear isomeric transition has recently been directly laser excited [1,2] and measured with high spectroscopic precision [3]. Nuclear clocks based on this transition are expected to be more robust [4,5] than and may outperform [6,7] current optical atomic clocks. They also promise sensitive tests for new physics beyond the standard model [5,8,9]. In light of these important advances and applications, a dramatic increase in the need for $^{229}$Th spectroscopy targets in a variety of platforms is anticipated. However, the growth and handling of high-concentration $^{229}$Th-doped crystals [5] used in previous measurements [1-3,10] are challenging due to the scarcity and radioactivity of the $^{229}$Th material. Here, we demonstrate a potentially scalable solution to these problems by demonstrating laser excitation of the nuclear transition in $^{229}$ThF$_4$ thin films grown with a physical vapor deposition process, consuming only micrograms of $^{229}$Th material. The $^{229}$ThF$_4$ thin films are intrinsically compatible with photonics platforms and nanofabrication tools for integration with laser sources and detectors, paving the way for an integrated and field-deployable solid-state nuclear clock with radioactivity up to three orders of magnitude smaller than typical \thor-doped crystals [1-3,10]. The high nuclear emitter density in $^{229}$ThF$_4$ also potentially enables quantum optics studies in a new regime. Finally, we describe the operation and present the estimation of the performance of a nuclear clock based on a defect-free ThF$_4$ crystal., Comment: 15 pages, 3 figures

LiSrAlF$_6$ crystals doped with $^{229}$Th are used in a laser-based search for the nuclear isomeric transition. Two spectroscopic features near the nuclear transition energy are observed. The first is a broad excitation feature that produces red-shifted fluorescence that decays with a timescale of a few seconds. The second is a narrow, laser-linewidth-limited spectral feature at $148.38219(4)_{\textrm{stat}}(20)_{\textrm{sys}}$ nm ($2020407.3(5)_{\textrm{stat}}(30)_{\textrm{sys}}$ GHz) that decays with a lifetime of $568(13)_{\textrm{stat}}(20)_{\textrm{sys}}$ s. This feature is assigned to the excitation of the $^{229}$Th nuclear isomeric state, whose energy is found to be $8.355733(2)_{\textrm{stat}}(10)_{\textrm{sys}}$ eV in $^{229}$Th:\thor:LiSrAlF$_6$., Comment: Submitted to Physical Review Letters on March 25, 2024

The Stark-interference technique is commonly used to amplify the feeble parity-violating signal in atomic experiments. As a result, interpretation of these experiments in terms of electroweak observables requires knowledge of the Stark-induced $E1$ transition amplitudes or, equivalently, transition polarizabilities. While the literature assumes that these transition polarizabilities do not depend on the nuclear spin, here we prove the contrary. The nuclear spin dependence arises due to hyperfine mixing of atomic states and requires a third-order perturbation theory (one hyperfine interaction and two electric-dipole interactions) treatment. We demonstrate that the so far neglected {\em tensor} contribution appears in the transition polarizability and present numerical results for the nuclear-spin-dependent corrections to the $6S_{1/2}\rightarrow{7S_{1/2}}$ transition polarizability in $^{133}$Cs. We investigate the effect of these corrections to transition polarizabilities on the extraction of the $^{133}$Cs anapole moment from the Boulder experiment [Science 275, 1759 (1997)]. We also consider their effect on the extraction of the ratio between the scalar and vector transition polarizabilities from the measurements [Phys. Rev. A 55, 2 (1997)]. While the corrections are minor at the current level of experimental accuracy, our analysis provides a framework for future experiments., Comment: 11 pages, 1 figure

Extracting electroweak observables from experiments on atomic parity violation (APV) using the Stark interference technique requires accurate knowledge of transition polarizabilities. In cesium, the focus of our paper, the $6S_{1/2}\rightarrow{7S_{1/2}}$ APV amplitude is deduced from the measured ratio of the APV amplitude to the vector transition polarizability, $\beta$. This ratio was measured with a $0.35\%$ uncertainty by the Boulder group [Science 275, 1759 (1997)]. Currently, there is a sizable discrepancy in different determinations of $\beta$ critically limiting the interpretation of the APV measurement. The most recent value [Phys. Rev. Lett. 123, 073002 (2019)] of $\beta=27.139(42)\, \mathrm{a.u.}$ was deduced from a semi-empirical sum-over-state determination of the scalar transition polarizability $\alpha$ and the measured $\alpha/\beta$ ratio [Phys. Rev. A 55, 1007 (1997)]. This value of $\beta$, however, differs by $\sim 0.7\%$ or $2.8\sigma$ from the previous determination of $\beta=26.957(51)$ by [Phys. Rev. A 62, 052101 (2000)] based on the measured ratio $M1/\beta$ of the magnetic-dipole $6S_{1/2}\rightarrow{7S_{1/2}}$ matrix element to $\beta$. Here, we revise the determination of $\beta$ by [Phys. Rev. Lett. 123, 073002 (2019)], using a more consistent and more theoretically complete treatment of contributions from the excited intermediate states in the sum-over-state $\alpha/\beta$ method. Our result of $\beta=26.887(38)\, \mathrm{a.u.}$ resolves the tension between the $\alpha/\beta$ and $M1/\beta$ approaches. We recommend the value of $\beta=26.912(30)$ obtained by averaging our result and that of [Phys. Rev. A 62, 052101 (2000)]., Comment: 9 pages, 2 figures v2: Reference added, small cosmetic changes to the text

We compute the reduced electric-dipole matrix elements $\langle{nS_{1/2}}||D||{n'P_J}\rangle$ with $n=6,7$ and $n'=6,7,\ldots,12$ in cesium using the most complete to date ab initio relativistic coupled-cluster method which includes singles, doubles, perturbative core triples, and valence triples. Our results agree with previous calculations at the linearized single double level but also show large contributions from nonlinear singles and doubles as well as valence triples. We also calculate the normalized ratio $\xi_{n,n'}\equiv(1/\sqrt{2})\langle{nS_{1/2}}||D||{n'P_{1/2}}\rangle/\langle{nS_{1/2}}||D||{n'P_{3/2}}\rangle$ which is important for experimental determination of matrix elements. The ratios $\xi_{6,n}$ display large deviations from the nonrelativistic limit which we associate with Cooper-like minima. Several appendices are provided where we document the procedure for constructing finite basis sets and our implementation of the random phase approximation and Brueckner-orbitals method., Comment: 26 pages, 17 figures v.2: uncertainties for removal energies provided, further comments and additional references added, typos corrected

We consider the implication of the recent measurement of the W-boson mass $M_W$ [Science 376, 170 (2022)] for atomic parity violation experiments. We show that the change in $M_W$ shifts the Standard Model prediction for the ${}^{133}$Cs nuclear weak charge to $Q_W({}^{133}{\rm Cs})=-72.85(6)$, i.e. by $5.5\sigma$ from its current value. This brings existing experimental result for $Q_W({}^{133}{\rm Cs})$ into an essential agreement with the Standard Model. Using our revised value for $Q_W({}^{133}{\rm Cs})$, we readjust constraints on physics beyond the Standard Model., Comment: 5 pages, 1 figure. v2: typo corrected, additional references added. v3: additional references added

We formulate a parity-mixed coupled-cluster (PM-CC) approach for high-precision calculations of parity non-conserving amplitudes in mono-valent atoms. Compared to the conventional formalism which uses parity-proper (PP) one-electron orbitals, the PM-CC method is built using parity-mixed (PM) orbitals. The PM orbitals are obtained by solving the Dirac-Hartree-Fock equation with the electron-nucleus electroweak interaction included (PM-DHF). There are several advantages to such a PM-CC formulation: (i) reduced role of correlations, as for the most experimentally-accurate to date ${}^{133}{\rm Cs}\,$ $6S_{1/2}-7S_{1/2}$ transition, the PM-DHF result is only 3% away from the accurate many-body value, while the conventional DHF result is off by 18%; (ii) avoidance of directly summing over intermediate states in expressions for parity non-conserving amplitudes which reduces theoretical uncertainties associated with highly-excited and core-excited intermediate states, and (iii) relatively straightforward upgrade of existing and well-tested large-scale PP-CC codes. We reformulate the CC method in terms of the PM-DHF basis and demonstrate that the cluster amplitudes are complex numbers with opposite parity real and imaginary parts. We then use this fact to map out a strategy through which the new PM-CC scheme may be implemented., Comment: 24 pages, 2 figures, 2 tables

We calculate the cross-sections of atomic ionization by absorption of scalar particles in the energy range from a few eV to 100 keV. We consider both nonrelativistic particles (dark matter candidates) and relativistic particles which may be produced inside Sun. We provide numerical results for atoms relevant for direct dark matter searches (O, Na, Ar, Ca, Ge, I, Xe, W and Tl). We identify a crucial flaw in previous calculations and show that they overestimated the ionization cross sections by several orders of magnitude due to violation of the orthogonality of the bound and continuum electron wave functions. Using our computed cross-sections, we interpret the recent data from the Xenon1T experiment, establishing the first direct bounds on coupling of scalars to electrons. We argue that the Xenon1T excess can be explained by the emission of scalars from the Sun. While our finding is in a similar tension with astrophysical bounds as the solar axion hypothesis, we establish direct limits on scalar DM for the $\sim 1-10\,\mathrm{keV}$ mass range. We also update axio-ionization cross-sections. Numerical data files are provided., Comment: 7 pages, 5 figures. 2nd version: appendix added, citations added, data files included. 3rd version: new results for CaOW_4 added

In heavy atoms and ions, nuclear structure effects are significantly enhanced due to the overlap of the electron wave functions with the nucleus. This overlap rapidly increases with the nuclear charge $Z$. We study the energy level shifts induced by the electric dipole and electric quadrupole nuclear polarization effects in atoms and ions with $Z \geq 20$. The electric dipole polarization effect is enhanced by the nuclear giant dipole resonance. The electric quadrupole polarization effect is enhanced because the electrons in a heavy atom or ion move faster than the rotation of the deformed nucleus, thus experiencing significant corrections to the conventional approximation in which they `see' an averaged nuclear charge density. The electric nuclear polarization effects are computed numerically for $1s$, $2s$, $2p_{1/2}$ and high $ns$ electrons. The results are fitted with elementary functions of nuclear parameters (nuclear charge, mass number, nuclear radius and deformation). We construct an effective potential which models the energy level shifts due to nuclear polarization. This effective potential, when added to the nuclear Coulomb interaction, may be used to find energy level shifts in multi-electron ions, atoms and molecules. The fitting functions and effective potentials of the nuclear polarization effects are important for the studies of isotope shifts and nonlinearity in the King plot which are now used to search for new interactions and particles., Comment: 17 pages, 3 figures, 10 tables

We demonstrate that electron electric dipole moment experiments with molecules in paramagnetic state are sensitive to $P,T$-violating nuclear forces and other $CP$-violating parameters in the hadronic sector. These experiments, in particular, measure the coupling constant $C_{SP}$ of the $CP$-odd contact semileptonic interaction. We establish relations between $C_{SP}$ and different $CP$-violating hadronic parameters including strength constants of the $CP$-odd nuclear potentials, $CP$-odd pion-nucleon interactions, quark-chromo EDM and QCD vacuum angle. These relations allow us to find limits on various $CP$-odd hadronic parameters., Comment: 13 pages. arXiv admin note: text overlap with arXiv:2004.10359

Experiments with paramagnetic ground or metastable excited states of molecules (ThO, HfF$^+$, YbF, YbOH, BaF, PbO, etc.) provide strong constraints on electron electric dipole moment (EDM) and coupling constant $C_{SP}$ of contact semileptonic interaction. We compute new contributions to $C_{SP}$ arising from the nucleon EDMs due to combined electric and magnetic electron-nucleon interaction. This allows us to improve limits from the experiments with paramagnetic molecules on the $CP$-violating parameters, such as the proton EDM, $|d_p|< 1.1\times 10^{-23} e\cdot $cm, the QCD vacuum angle, $|\bar \theta|<1.4\times 10^{-8}$, as well as the quark chromo-EDMs and $\pi$-meson-nucleon couplings. Our results may also be used to search for the axion dark matter which produces oscillating $\bar\theta$., Comment: 27 pages. V2: major corrections, V3: comments on uncertainties and other minor corrections, journal version

We show that existing calculations of the interaction between nuclear Schiff moments and electrons in molecules use an inaccurate operator which gives rise to significant errors. By comparing the matrix elements of the accurate and imprecise Schiff moment operators, we calculated the correction factor as a function of the nuclear charge Z and presented corrected results for the T,P-violating interaction of the nuclear spin with the molecular axis in the TlF, RaO, PbO, TlCN, ThO, AcF molecules and in the ferroelectric solid PbTiO$_3$., Comment: 4 pages, 1 figure

The interaction of standard model's particles with the axionic Dark Matter field may generate oscillating nuclear electric dipole moments (EDMs), oscillating nuclear Schiff moments and oscillating nuclear magnetic quadrupole moments (MQMs) with a frequency corresponding to the axion's Compton frequency. Within an atom or a molecule an oscillating EDM, Schiff moment or MQM can drive transitions between atomic or molecular states. The excitation events can be detected, for example, via subsequent fluorescence or photoionization. Here we calculate the rates of such transitions. If the nucleus has octupole deformation or quadrupole deformation then the transition rate due to Schiff moment and MQM can be up to $10^{-16}$ transition per molecule per year. In addition, an MQM-induced transition may be of M2-type, which is useful for the elimination of background noise since M2-type transitions are suppressed for photons., Comment: 10 pages

According to the Schiff theorem nuclear electric dipole moment (EDM) is completely shielded in a neutral atom by electrons. This makes a static nuclear electric dipole moment (EDM) unobservable. Interaction with the axion dark matter field generates nuclear EDM $d=d_0 \cos (\omega t)$ oscillating with the frequency $\omega= m_a c^2/\hbar$ . This EDM generates atomic EDM proportional to $\omega^2$. This effect is strongly enhanced in molecules since nuclei move slowly and do not produce as efficient screening of oscillating nuclear EDM as electrons do. An additional strong enhancement comes due to a small energy interval between rotational molecular levels. Finally, if the nuclear EDM oscillation frequency is in resonance with a molecular transition, there may be a significant resonance enhancement., Comment: 8 pages, 2 figures

Dark photon is a massive vector particle which couples to the physical photon through the kinetic mixing term. Such particles, if exist, are produced in photon beams and, in particular, in laser radiation. Due to the oscillations between the physical photon and the dark photon, the latter may be, in principle, detected in the light-shining-through-a-wall experiment. We propose a variant of this experiment where the detection of dark photons is based on the atomic transitions. The key feature of this scheme is that the detection probability is first order in the coupling constant due to the interference term in the photon and dark photon absorption amplitudes. We expect that such experiment may give new constraints on dark photon coupling constant in the mass region $10^{-3}< m < 10^{-2}$ eV., Comment: 8 pages

According to the Schiff theorem, the atomic electrons completely screen the atomic nucleus from an external static electric field. However, this is not the case if the field is time-dependent. Electronic orbitals in atoms either shield the nucleus from an oscillating electric field when the frequency of the field is off the atomic resonances or enhance this field when its frequency approaches an atomic transition energy. In molecules, not only electronic, but also rotational and vibrational states are responsible for the screening of oscillating electric fields. As will be shown in this paper, the screening of a low-frequency field inside molecules is much weaker than it appears in atoms owing to the molecular ro-vibrational states. We systematically study the screening of oscillating electric fields inside diatomic molecules in different frequency regimes,i.e., when the field's frequency is either of order of ro-vibrational or electronic transition frequencies. In the resonance case, we demonstrate that the microwave-frequency electric field may be enhanced up to six orders in magnitude due to ro-vibrational states. We also derive the general formulae for the screening and resonance enhancement of oscillating electric field in polyatomic molecules. Possible applications of these results include nuclear electric dipole moment measurements and stimulation of nuclear reactions by laser light., Comment: 14 pages, 1 figure

In this paper, we show that in the vicinity of certain astronomical bodies, e.g., a Neutron Star, a Black Hole, there exist significant enhancements of Dark Matter's density and current, due to its interaction with the gravitational field of the bodies. This enhancement implies that the effects of Dark Matter - Normal Matter interactions are enhanced and hence might be observable., Comment: 9 pages, 18 figures

In certain laboratory experiments the production and/or detection of axions is due to the photon-axion transformations in a strong magnetic field. This process is coherent, and the rate of the transformation is proportional to the length $l$ and magnitude $B$ of the magnetic field squared, $\sim l^2B^2$. In the present paper, we consider coherent production of axions due to the forward scattering of photons on atoms or molecules. This process may be represented as being due to an effective electromagnetic field which converts photons to axions. We present analytical expressions for such effective magnetic and electric fields induced by resonant atomic M0 and M1 transitions, as well as give some numerical estimates for these fields. The corresponding experiments would allow one to measure the electron-axion coupling constant $g_{ae}$ in the same way as the photon-axion coupling $g_{a\gamma}$ is studied., Comment: 6 pages

Detection schemes for the quantum chromodynamics axions and other axion-like particles in light-shining-through-a-wall (LSW) experiments are based on the conversion of these particles into photons in a magnetic field. An alternative scheme may involve the detection via a resonant atomic or molecular transition induced by resonant axion absorption. The signal obtained in this process is second order in the axion-electron interaction constant but may become first order if we allow interference between the axion-induced transition amplitude and the transition amplitude induced by the electromagnetic radiation that produces the axions., Comment: 12 pages, 4 figures, 3 tables