Search

Most dark matter searches to date employ a single sensor for detection. In this chapter, we explore the power of distributed networks in dark matter searches. Compared to a single sensor, networks offer several advantages, such as the ability to probe spatiotemporal signatures of the putative signal and, as a result, an improved rejection of false positives, better sensitivity, and improved confidence in the dark matter origin of the sought-after signal. We illustrate our general discussion with two examples: (1) the Global Network of Optical Magnetometers for Exotic physics searches (GNOME) and (2) the constellation of atomic clocks on board satellites of the Global Positioning System (GPS).

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., 7 pages, 5 figures. 2nd version: appendix added, citations added, data files included. 3rd version: new results for CaOW_4 added

Results are reported from the first full-scale search for transient signals from exotic fields of astrophysical origin using data from a newly constructed Earth-scale detector: the Global Network of Optical Magnetometers for Exotic physics searches (GNOME). Data collected by the GNOME consist of correlated measurements from optical atomic magnetometers located in laboratories all over the world. GNOME data are searched for patterns of signals propagating through the network consistent with exotic fields composed of ultralight bosons such as axion-like particles (ALPs). Analysis of data from a continuous month-long operation of the GNOME finds no statistically significant signals consistent with those expected due to encounters with topological defects (axion domain walls), placing new experimental constraints on such dark matter scenarios.

Ultralight bosons such as axion-like particles are viable candidates for dark matter. They can form stable, macroscopic field configurations in the form of topological defects that could concentrate the dark matter density into many distinct, compact spatial regions that are small compared with the Galaxy but much larger than the Earth. Here we report the results of the search for transient signals from the domain walls of axion-like particles by using the global network of optical magnetometers for exotic (GNOME) physics searches. We search the data, consisting of correlated measurements from optical atomic magnetometers located in laboratories all over the world, for patterns of signals propagating through the network consistent with domain walls. The analysis of these data from a continuous month-long operation of GNOME finds no statistically significant signals, thus placing experimental constraints on such dark matter scenarios., A search for transient dark matter in the form of domain walls of axion-like particles finds no statistically significant signal. This places constraints on our theoretical understanding of such scenarios.

Multi-messenger astronomy, the coordinated observation of different classes of signals originating from the same astrophysical event, provides a wealth of information about astrophysical processes with far-reaching implications. So far, the focus of multi-messenger astronomy has been the search for conventional signals from known fundamental forces and standard model particles, like gravitational waves (GW). In addition to these known effects, quantum sensor networks could be used to search for astrophysical signals predicted by beyond-standard-model (BSM) theories. Exotic bosonic fields are ubiquitous features of BSM theories and appear while seeking to understand the nature of dark matter and dark energy and solve the hierarchy and strong CP problems. We consider the case where high-energy astrophysical events could produce intense bursts of exotic low-mass fields (ELFs). We propose to expand the toolbox of multi-messenger astronomy to include networks of precision quantum sensors that by design are shielded from or insensitive to conventional standard-model physics signals. We estimate ELF signal amplitudes, delays, rates, and distances of GW sources to which global networks of atomic magnetometers and atomic clocks could be sensitive. We find that, indeed, such precision quantum sensor networks can function as ELF telescopes to detect signals from sources generating ELF bursts of sufficient intensity. Thus ELFs, if they exist, could act as additional messengers for astrophysical events., 19 pages, 5 figures

Highly charged ions (HCIs) are promising candidates for the next generation of atomic clocks, owing to their tightly bound electron cloud, which significantly suppresses the common environmental disturbances to the quantum oscillator. Here we propose and pursue an experimental strategy that, while focusing on various HCIs of a single atomic element, keeps the number of candidate clock transitions as large as possible. Following this strategy, we identify four adjacent charge states of nickel HCIs that offer as many as six optical transitions. Experimentally, we demonstrated the essential capability of producing these ions in the low-energy compact Shanghai-Wuhan Electron Beam Ion Trap. We measured the wavelengths of four magnetic-dipole ($M$1) and one electric-quadrupole ($E$2) clock transitions with an accuracy of several ppm with a novel calibration method; two of these lines were observed and characterized for the first time in controlled laboratory settings. Compared to the earlier determinations, our measurements improved wavelength accuracy by an order of magnitude. Such measurements are crucial for constraining the range of laser wavelengths for finding the "needle in a haystack" narrow lines. In addition, we calculated frequencies and quality factors, evaluated sensitivity of these six transitions to the hypothetical variation of the electromagnetic fine structure constant $\alpha$ needed for fundamental physics applications. We argue that all the six transitions in nickel HCIs offer intrinsic immunity to all common perturbations of quantum oscillators, and one of them has the projected fractional frequency uncertainty down to the remarkable level of 10$^{-19}$., Comment: To be published in Physical Review A

We conduct frequency comparisons between a state-of-the-art strontium optical lattice clock, a cryogenic crystalline silicon cavity, and a hydrogen maser to set new bounds on the coupling of ultralight dark matter to Standard Model particles and fields in the mass range of $10^{-16}$ $-$ $10^{-21}$ eV. The key advantage of this two-part ratio comparison is the differential sensitivities to time variation of both the fine-structure constant and the electron mass, achieving a substantially improved limit on the moduli of ultralight dark matter, particularly at higher masses than typical atomic spectroscopic results. Furthermore, we demonstrate an extension of the search range to even higher masses by use of dynamical decoupling techniques. These results highlight the importance of using the best performing atomic clocks for fundamental physics applications as all-optical timescales are increasingly integrated with, and will eventually supplant, existing microwave timescales., 11 pages, 10 figures

Author(s): Xiao, Di; Li, Jiguang; Campbell, Wesley C; Dellaert, Thomas; McMillin, Patrick; Ransford, Anthony; Roman, Conrad; Derevianko, Andrei | Abstract: 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 to use an alternative system to resolve this tension, a singly charged ion of the same $^{173}\mathrm{Yb}$ isotope. Utilizing the substantial suite of tools developed around $\mathrm{Yb}^+$ for quantum information applications, we propose to extract nuclear octupole and hexadecapole moments from measuring hyperfine splittings in the extremely long lived first excited state ($4f^{13}(^2\!F^{o})6s^2$, $J=7/2$) of $^{173}\mathrm{Yb}^+$. We present results of atomic structure calculations in support of the proposed measurements.

Cosmological observations indicate that 85% of all matter in the Universe is dark matter (DM), yet its microscopic composition remains a mystery. One hypothesis is that DM arises from ultralight quantum fields that form macroscopic objects such as topological defects. Here we use GPS as a ~ 50,000 km aperture DM detector to search for such defects in the form of domain walls. GPS navigation relies on precision timing signals furnished by atomic clocks hosted on board GPS satellites. As the Earth moves through the galactic DM halo, interactions with topological defects could cause atomic clock glitches that propagate through the GPS satellite constellation at galactic velocities ~ 300 km/s. Mining 16 years of archival GPS data, we find no evidence for DM in the form of domain walls at our current sensitivity level. This allows us to improve the limits on certain quadratic scalar couplings of domain wall DM to standard model particles by several orders of magnitude., 7 pages (main text), and 12 pages for Supplementary Information. v3: Update title

The Gamma Factory initiative proposes to develop novel research tools at CERN by producing, accelerating and storing highly relativistic, partially stripped ion beams in the SPS and LHC storage rings. By exciting the electronic degrees of freedom of the stored ions with lasers, high-energy narrow-band photon beams will be produced by properly collimating the secondary radiation that is peaked in the direction of ions' propagation. Their intensities, up to $10^{17}$ photons per second, will be several orders of magnitude higher than those of the presently operating light sources in the particularly interesting $\gamma$--ray energy domain reaching up to 400 MeV. This article reviews opportunities that may be afforded by utilizing the primary beams for spectroscopy of partially stripped ions circulating in the storage ring, as well as the atomic-physics opportunities afforded by the use of the secondary high-energy photon beams. The Gamma Factory will enable ground breaking experiments in spectroscopy and novel ways of testing fundamental symmetries of nature., Comment: 15 pages, 3 figures

International audience; The Gamma Factory (GF) initiative proposes to use partially stripped ion (PSI) beams as drivers of a new type of high-intensity and high-energy (0.1–400 MeV) photon source. As part of the ongoing Physics Beyond Collider studies, initial beam tests were carried out in 2017 and 2018 at the SPS and LHC with partially stripped xenon and lead beams. This contribution discusses the results of these tests and the preparations for the next GF R&D step: the proof-of-principle experiment at the SPS to study interaction of PSI beams with the laser light

Acta physica Polonica / B / Proceedings supplement 13(4), 645 (2020). doi:10.5506/APhysPolBSupp.13.645, Published by Inst. of Physics, Jagellonian Univ., Cracow

”DArk Matter from Non Equal Delays” (DAMNED) is a new experiment that aims to check for space or time variation of physics fundamental constants. This 3 arm Mach-Zender experiment allows us to compare an ultra-stable cavity to itself in the past through the delay created by a multi kilometer long optical fiber. A massive scalar dark matter field (DM) would be seen on the experiment beat and we aim to constrain a new combination of the DM coupling constants.

We discuss the possibility of creating novel research tools by producing and storing highly relativistic beams of highly ionised atoms in the CERN accelerator complex, and by exciting their atomic degrees of freedom with lasers to produce high-energy photon beams. Intensity of such photon beams would be by several orders of magnitude higher than offered by the presently operating light sources, in the particularly interesting gamma-ray energy domain of 0.1-400 MeV. In this energy range, the high-intensity photon beams can be used to produce secondary beams of polarised electrons, polarised positrons, polarised muons, neutrinos, neutrons and radioactive ions. New research opportunities in a wide domain of fundamental and applied physics can be opened by the Gamma Factory scientific programme based on the above primary and secondary beams., 12 pages; presented by W. Placzek at the XXV Cracow Epiphany Conference on Advances in Heavy Ion Physics, 8-11 January 2019, Cracow, Poland

Black-body radiation (BBR) shifts of $^3\!P_0-^1\!S_0$ clock transition in divalent atoms Cd and Zn are evaluated using accurate relativistic many-body techniques of atomic structure. Static polarizabilities of the clock levels and relevant electric-dipole matrix elements are computed. We also present a comparative overview of the BBR shifts in optical clocks based on neutral divalent atoms trapped in optical lattices.

There are several networks of precision quantum sensors in existence, including networks of atomic clocks, magnetometers, and gravitational wave detectors. These networks can be re-purposed for searches of exotic physics, such as direct dark matter searches. Here we explore a detection strategy for macroscopic dark matter objects with such networks using the matched-filter technique. Such "clumpy" dark matter objects would register as transients sweeping through the network at galactic velocities. As a specific example, we consider a network of atomic clocks aboard the Global Positioning System (GPS) satellites. We apply the matched-filter technique to simulated GPS atomic clock data and study its utility and performance. The analysis and the developed methodology have a wide applicability to other networks of quantum sensors., Comment: 19 pages, 9 figures

We discuss the use of optical cavities as tools to search for dark matter (DM) composed of virialized ultra-light fields (VULFs). Such fields could lead to oscillating fundamental constants, resulting in oscillations of the length of rigid bodies. We propose searching for these effects via differential strain measurement of rigid and suspended-mirror cavities. We estimate that more than two orders of magnitude of unexplored phase space for VULF DM couplings can be probed at VULF Compton frequencies in the audible range of 0.1-10 kHz., 6 pages, 4 figures, title updated

A method is proposed to detect some candidates of dark matter with a network of precision-measurement devices such as atomic clocks. Spatiotemporal correlation functions of the ultralight dark-matter fields are derived for formalizing the proposed scheme.

We analyze the prospects of employing a distributed global network of precision measurement devices as a dark matter and exotic physics observatory. In particular, we consider the atomic clocks of the Global Positioning System (GPS), consisting of a constellation of 32 medium-Earth orbit satellites equipped with either Cs or Rb microwave clocks and a number of Earth-based receiver stations, some of which employ highly-stable H-maser atomic clocks. High-accuracy timing data is available for almost two decades. By analyzing the satellite and terrestrial atomic clock data, it is possible to search for transient signatures of exotic physics, such as "clumpy" dark matter and dark energy, effectively transforming the GPS constellation into a 50,000km aperture sensor array. Here we characterize the noise of the GPS satellite atomic clocks, describe the search method based on Bayesian statistics, and test the method using simulated clock data. We present the projected discovery reach using our method, and demonstrate that it can surpass the existing constrains by several order of magnitude for certain models. Our method is not limited in scope to GPS or atomic clock networks, and can also be applied to other networks of precision measurement devices., See also Supplementary Information located in ancillary files

Atomic clocks reached a record-breaking uncertainty of less than 10−18 and the time needed to compare clocks is now less than an hour. These results push towards a possible redefinition of the second from a microwave to an optical standard. Atomic clocks reached a record-breaking uncertainty of less than 10−18 and the time needed to compare clocks is now less than an hour. These results push towards a possible redefinition of the second from a microwave to an optical standard.

We explore the feasibility of a compact high-precision Hg atomic clock based on a hollow core optical fiber. We evaluate the sensitivity of the $^1S_0$-$^3P_0$ clock transition in Hg and other divalent atoms to the fiber inner core surface at non-zero temperatures. The Casimir-Polder interaction induced $^1S_0$-$^3P_0$ transition frequency shift is calculated for the atom inside the hollow capillary as a function of atomic position, capillary material, and geometric parameters. For $^{199}\mathrm{Hg}$ atoms on the axis of a silica capillary with inner radius $\geq 15 \,\mu \mathrm{m}$ and optimally chosen thickness $d\sim 1 \,\mu \mathrm{m}$, the atom-surface interaction induced $^1S_0$-$^3P_0$ clock transition frequency shift can be kept on the level $\delta\nu/\nu_{\mathrm{Hg}} \sim10^{-19}$. We also estimate the atom loss and heating due to the collisions with the buffer gas, lattice intensity noise induced heating, spontaneous photon scattering, and residual birefringence induced frequency shifts., Comment: 8 pages, 5 figures, submitted

We tabulate spontaneous emission rates for all possible 811 electric-dipole-allowed transitions between the 75 lowest-energy states of Ca I. These involve the $4sns$ ($n=4-8$), $4snp$ ($n=4-7$), $4snd$ ($n=3-6$), $4snf$ ($n=4-6$), $4p^2$, and $3d4p$ electronic configurations. We compile the transition rates by carrying out ab initio relativistic calculations using the combined method of configuration interaction and many-body perturbation theory. The results are compared to the available literature values. The tabulated rates can be useful in various applications, such as optimizing laser cooling in magneto-optical traps, estimating various systematic effects in optical clocks and evaluating static or dynamic polarizabilities and long-range atom-atom interaction coefficients and related atomic properties., Comment: 33 pages

We propose a protocol for creating a fully entangled Greenberger-Horne-Zeilinger-type state of neutral atoms in spatially separated optical atomic clocks. In our scheme, local operations make use of the strong dipole-dipole interaction between Rydberg excitations, which give rise to fast and reliable quantum operations involving all atoms in the ensemble. The necessary entanglement between distant ensembles is mediated by single-photon quantum channels and collectively enhanced light-matter couplings. These techniques can be used to create the recently proposed quantum clock network based on neutral atom optical clocks. We specifically analyze a possible realization of this scheme using neutral Yb ensembles.

We demonstrate that the coherence of a single mobile atomic qubit can be well preserved during a transfer process among different optical dipole traps (ODTs). This is a prerequisite step in realizing a large-scale neutral atom quantum information processing platform. A qubit encoded in the hyperfine manifold of $^{87}$Rb atom is dynamically extracted from the static quantum register by an auxiliary moving ODT and reinserted into the static ODT. Previous experiments were limited by decoherences induced by the differential light shifts of qubit states. Here we apply a magic-intensity trapping technique which mitigates the detrimental effects of light shifts and substantially enhances the coherence time to $225 \pm 21\,\mathrm{ms}$. The experimentally demonstrated magic trapping technique relies on the previously neglected hyperpolarizability contribution to the light shifts, which makes the light shift dependence on the trapping laser intensity to be parabolic. Because of the parabolic dependence, at a certain "magic" intensity, the first order sensitivity to trapping light intensity variations over ODT volume is eliminated. We experimentally demonstrate the utility of this approach and measure hyperpolarizability for the first time. Our results pave the way for constructing a scalable quantum-computing architectures with single atoms trapped in an array of magic ODTs., 6 pages, 5 figures

Recently invented and demonstrated, optical lattice clocks hold great promise for improving the precision of modern timekeeping. These clocks aim at the 10^-18 fractional accuracy, which translates into a clock that would neither lose or gain a fraction of a second over an estimated age of the Universe. In these clocks, millions of atoms are trapped and interrogated simultaneously, dramatically improving clock stability. Here we discuss the principles of operation of these clocks and, in particular, a novel concept of "magic" trapping of atoms in optical lattices. We also highlight recently proposed microwave lattice clocks and several applications that employ the optical lattice clocks as a platform for precision measurements and quantum information processing., 18 pages, 15 figures

The electric dipole polarizabilities evaluated at imaginary frequencies for hydrogen, the alkali-metal atoms, the alkaline earth atoms, and the inert gases are tabulated along with the resulting values of the atomic static polarizabilities, the atom-surface interaction constants, and the dispersion (or van der Waals) constants for the homonuclear and the heteronuclear diatomic combinations of the atoms.

We predict the possibility of "triply-magic" optical lattice trapping of neutral divalent atoms. In such a lattice, the ${^1}\!S_{0}$ and ${^3}\!P_{0}$ clock states and an additional Rydberg state experience identical optical potentials, fully mitigating detrimental effects of the motional decoherence. In particular, we show that this triply magic trapping condition can be satisfied for Yb atom at optical wavelengths and for various other divalent systems (Ca, Mg, Hg and Sr) in the UV region. We assess the quality of triple magic trapping conditions by estimating the probability of excitation out of the motional ground state as a result of the excitations between the clock and the Rydberg states. We also calculate trapping laser-induced photoionization rates of divalent Rydberg atoms at magic frequencies. We find that such rates are below the radiative spontaneous-emission rates, due to the presence of Cooper minima in photoionization cross-sections.

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 nonvanishing 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 apply the results of the calculation to microwave atomic clocks where the coupling of atomic quadrupole moments to gradients of electric fields leads to clock frequency uncertainties. We show that for $^{133}\text{Cs}$ atomic clocks, the spatial gradients of electric fields must be smaller than $30\phantom{\rule{0.28em}{0ex}}\mathrm{V}/{\mathrm{cm}}^{2}$ to guarantee fractional inaccuracies below ${10}^{\ensuremath{-}16}$.

We discuss the use of atom interferometry as a tool to search for Dark Matter (DM) composed of ultra-light scalar fields. Previous work on ultra-light DM detection using accelerometers has considered the possibility of equivalence principle violating effects whereby gradients in the dark matter field can directly produce relative accelerations between media of differing composition. In atom interferometers, we find that time-varying phase signals from oscillatory, or dilaton-like, DM can also arise due to changes in the atom rest mass that can occur between light-pulses throughout the interferometer sequence as well as changes in the earth's gravitational field. We estimate that several orders of magnitude of unexplored phase space for light DM fields can be probed with our proposed method., Comment: 5 pages, 2 figures, typos corrected, referee comments included, main results unchanged

We study the effect of resonances associated with complex molecular interaction of Rydberg atoms on Rydberg blockade. We show that densely-spaced molecular potentials between doubly-excited atomic pairs become unavoidably resonant with the optical excitation at short interatomic separations. Such molecular resonances limit the coherent control of individual excitations in Rydberg blockade. As an illustration, we compute the molecular interaction potentials of Rb atoms near the $100s$ states asymptote to characterize such detrimental molecular resonances, determine the resonant loss rate to molecules and inhomogeneous light shifts. Techniques to avoid the undesired effect of molecular resonances are discussed., Comment: 5 pages + supplementary materials

Postulating the existence of a fnite-mass mediator of T,P-odd coupling between atomic electrons and nucleons we consider its effect on permanent electric dipole moment (EDM) of diamagnetic atoms. We present both numerical and analytical analysis for such mediator-induced EDMs and compare it with EDM results for the conventional contact interaction. Based on this analysis we derive limits on coupling strengths and carrier masses from experimental limits on EDM of 199Hg atom.

The static and dynamic electric dipole, quadrupole, and octupole polarizabilities of the alkaline-earth atoms (beryllium, magnesium, calcium, strontium, and barium) in the ground state were calculated. The dynamic polarizabilities obtained were used to calculate the van der Waals coefficients C 6, C 8, and C 10 of alkaline-earth metal dimers for the interaction of two like atoms in the ground state. The results are compared with other theoretical and experimental data.

We consider long-range interactions between two alkali-metal atoms in their respective ground states. We extend the previous relativistic many-body calculations of C_6 dispersion coefficients [Phys.Rev. Lett. {\bf 82}, 3589 (1999)] to higher-multipole coefficients C_8 and C_10. A special attention is paid to usually omitted contribution of core-excited states. We calculate this contribution within relativistic random-phase approximation and demonstrate that for heavy atoms core excitations contribute as much as 10% to the dispersion coefficients. We tabulate results for both homonuclear and heteronuclear dimers and estimate theoretical uncertainties. The estimated uncertainties for C_8 coefficients range from 0.5% for Li_2 to 4% for Cs_2., Comment: 12 pages, submitted to Journal of Chemical Physics

We evaluate the feasibility of using magnetic-dipole (M1) transitions in highly-charged ions as a basis of an optical atomic clockwork of exceptional accuracy. We consider a range of possibilities, including M1 transitions between clock levels of the same fine-structure and hyperfine-structure manifolds. In highly charged ions these transitions lie in the optical part of the spectra and can be probed with lasers. The most direct advantage of our proposal comes from the low degeneracy of clock levels and the simplicity of atomic structure in combination with negligible quadrupolar shift. We demonstrate that such clocks can have projected fractional accuracies below the $10^{-20}-10^{-21}$ level for all common systematic effects, such as black-body radiation, Zeeman, AC-Stark and quadrupolar shifts. Notice that usually-employed hyperfine clock transitions lie in the microwave spectral region. Our proposal moves such transitions to the optical domain. As the hyperfine transition frequencies depend on the fine-structure constant, electron-to-proton mass ratio, and nuclear magnetic moment, our proposal expands the range of experimental schemes for probing space and time variations of fundamental constants., 5 pages, 1 figure, accepted in PRL

We calculate the potential energy curves, the permanent dipole moment curves, and the lifetimes of the ground and excited vibrational states of the heteronuclear alkali dimers XY (X, Y = Li, Na, K, Rb, Cs) in the X1{\Sigma}+ electronic state using the coupled cluster with singles doubles and triples (CCSDT) method. All-electron quadruple-{\zeta} basis sets with additional core functions are used for Li and Na, and small-core relativistic effective core potentials with quadruple-{\zeta} quality basis sets are used for K, Rb and Cs. The inclusion of the coupled cluster non-perturbative triple excitations is shown to be crucial for obtaining the accurate potential energy curves. Large one-electron basis set with additional core functions is needed for the accurate prediction of permanent dipole moments. The dissociation energies are overestimated by only 14 cm-1 for LiNa and by no more than 114 cm-1 for the other molecules. The discrepancies between the experimental and calculated harmonic vibrational frequencies are less than 1.7 cm-1, and the discrepancies for the anharmonic correction are less than 0.1 cm-1. We show that correlation between atomic electronegativity differences and permanent dipole moment of heteronuclear alkali dimers is not perfect. To obtain the vibrational energies and wave functions the vibrational Schr\"odinger equation is solved with the B-spline basis set method. The transition dipole moments between all vibrational states, the Einstein coefficients and the lifetimes of the vibrational states are calculated. We analyze the decay rates of the vibrational states in terms of spontaneous emission, and stimulated emission and absorption induced by black body radiation. In all studied heteronuclear alkali dimers the ground vibrational states have much longer lifetimes than any excited states.

Laser cooling of atoms and molecules is an enabling technology for a number of applications, including atomic clocks, navigational sensors and quantum information processing. So far applications of this powerful technique have been limited to a handful of species as the conventional laser cooling requires closed (cycling) transitions. Here we will theoretically investigate the possibility of extending laser cooling techniques to a much wider class of multilevel atoms and molecules. The basic idea is to employ controllable coherent trains of laser pulses (frequency combs). Recently the power and spectral coverage of frequency combs have grown considerably with projected average powers above 10 kW. We will take advantage of this emerging technology. In the first project, we will exploit spectral selectivity of the combs and develop a time sequence protocol to move population across multiple levels with the goal of optimizing Doppler cooling for multi-level systems. In the second project, we will investigate stimulated optical force to slow heteronuclear molecules using ro-vibrational transitions inside the ground electronic state. Further, we propose to apply concepts from quantum-control and learning algorithms for finding optimal pulse sequences for cooling molecules even when the knowledge about their internal structures is imprecise.

Quantum-mechanical calculations of the potential energy curves of the singlet and triplet states of LiH, NaH, KH, RbH, and CsH formed by the approach of ground state alkali–metal atoms and hydrogen atoms are presented. Precise values are determined for the coefficients of the van der Waals interaction and estimates are made of the contribution of the exchange interaction at large distances. Together with empirical data, they are used to assess and improve the accuracy of the ab initio potentials.

We present a theoretical study of O(ka) and O(k2a2) corrections to the dipole approximation in photoionization of rare gas atoms, where k is the magnitude of the photon wave vector and a is the radius of the ionized subshell. In the dipole approximation, the photoelectron angular distribution is characterized by the single parameter β. The O(ka) corrections are characterized by two parameters γ and δ, and the O(k2a2) corrections are characterized by three parameters λ, μ, and ν, constrained by the relation λ + μ + ν = 0 and a correction Δβ to the dipole parameter β. Formulas are given for the non-dipole parameters in terms of reduced matrix elements of electric and magnetic multipole operators. Tables and graphs of the seven angular distribution parameters, calculated in the relativistic independent-particle approximation (IPA), are given for electron energies ranging from 20 to 5000 eV for all 41 subshells of the rare gas atoms He, Ne, Ar, Kr, and Xe. Tables and graphs of the O(ka) parameters are also given in the energy range 2–60 eV for the n = 3 and 4 shells of Kr, and for the n = 4 and 5 shells of Xe, where interesting non-dipole effects are found. Comparisons of the IPA calculations with correlated relativistic random-phase approximation calculations are made for selected subshells of Ar and Kr, illustrating the influence of correlation on the non-dipole parameters.

The influence of negative-energy states (NES) on forbidden magnetic-dipole $ns_{1/2}-(n+1)s_{1/2}$ transitions in alkali-metal atoms is investigated. We find that the NES contributions are significant in almost all cases and for rubidium reduce the transition rate by a factor of 8. We tabulate magnetic-dipole (M_1) transition amplitudes for the alkalis. Our M_1 value for cesium, where accurate measurements are available, differs from experiment by 16%. We briefly discuss the feasibility of an experimental test of NES effects., Comment: 4 pages 2 figures