Alkaline-earth Atoms Research Articles

SU(N) magnetism with ultracold molecules

Abstract Quantum systems with SU(N) symmetry are paradigmatic settings for quantum many-body physics. They have been studied for the insights they provide into complex materials and their ability to stabilize exotic ground states. Ultracold alkaline-earth atoms were predicted to exhibit SU(N) symmetry for N = 2I +1 = 1, 2, . . . , 10, where I is the nuclear spin. Subsequent experiments have revealed rich many-body physics. However, alkaline-earth atoms realize this symmetry only for fermions with repulsive interactions. In this paper, we predict that ultracold molecules shielded from destructive collisions with static electric fields or microwaves exhibit SU(N) symmetry, which holds because deviations of the s-wave scattering length from the spin-free values are only about 3% for CaF with static-field shielding and are estimated to be even smaller for bialkali molecules. They open the door to N as large as 32 for bosons and 36 for fermions. They offer important features unachievable with atoms, including bosonic systems and attractive interactions.

Slowing Down a Coherent Superposition of Circular Rydberg States of Strontium.

Rydberg alkaline earth atoms are promising tools for quantum simulation and metrology. When one of the two valence electrons is promoted to long-lived circular states, the second valence electron can be optically manipulated without significant autoionization. We harness this feature to demonstrate laser slowing of a thermal atomic beam of circular strontium atoms. By driving the main ion core 422nm wavelength resonance, we observe a velocity reduction of 50 m/s without significant autoionization. We also show that a superposition of circular states undergoes very weak decoherence during the cooling process, up to the scattering of more than 1000 photons. This robustness opens new perspectives for quantum simulations over long timescales with circular atoms, while simultaneously cooling their motional state. It makes it possible to mitigate the harmful effects of unavoidable heating due to spin-motion coupling during a quantum simulation.

Calcium single atoms stabilized by nitrogen coordination in metal–organic frameworks as efficient solid base catalysts

Considerable attention has been paid to the preparation of single-atom solid base catalysts (SASBCs) owing to their high activity and maximized utilization of basic sites. At present, the reported fabrication methods of SASBCs, such as two-step reduction strategy and sublimation capture strategy, require high temperature. Such a high activation temperature is easy to cause the sublimation loss of alkali or alkaline earth metal atoms and destructive to the support structure. Herein, a new SASBC, Ca1/UiO-67-BPY, is fabricated, in which the alkaline earth metal Ca sites are immobilized onto N-rich metal–organic framework UiO-67-BPY at room temperature. The results show that the atomic configuration of Ca single atoms is coordinated by two N atoms in the framework. The obtained Ca SASBC possesses ordered structure and exhibits high product yield of 87.2% in the Knoevenagel reaction between benzaldehyde and malononitrile. Furthermore, thanks to the Ca single atoms sites anchored on UiO-67-BPY, the Ca1/UiO-67-BPY catalyst also shows good stability during cycles. This work might offer new insight in designing SASBCs for different base-catalyzed reactions.

Light-element and purely charge-based topological materials

We examine a class of Hamiltonians characterized by interatomic, interorbital even-odd parity hybridization as a model for a family of topological insulators without the need for spin-orbit coupling. Non-trivial properties of these materials are exemplified by studying the topologically-protected edge states ofs-phybridized alkali and alkaline earth atoms in one and two-dimensional lattices. In 1D the topological features are analogous to the canonical Su-Schrieffer-Heeger model but, remarkably, occur in the absence of dimerization. Alkaline earth chains, with Be standing out due to its gap size and near particle-hole symmetry, are of particular experimental interest since their Fermi energy without doping lies directly at the level of topological edge states. Similar physics is demonstrated to occur in a 2D honeycomb lattice system ofs-pbonded atoms, where dispersive edge states emerge. Lighter elements are predicted using this model to host topological states in contrast to spin-orbit coupling-induced band inversion favoring heavier atoms.

Oxygen Atom Stabilization by a Main-Group Lewis Acid: Observation and Characterization of an OBeF2 Complex with a Triplet Ground State.

Terminal oxygen radicals involving p- and d-block atoms are quite common, but s-block compounds with an oxygen radical character remain rare. Here, we report that alkaline-earth metal beryllium atoms react with OF2 to form the oxygen beryllium fluorides OBeF and OBeF2. These species are characterized by matrix-isolation infrared spectroscopy with isotopic substitution and quantum-chemical calculations. The linear molecule OBeF has a 2Π ground state with an oxyl radical character. The 3A2 (C2v) ground state of OBeF2 represents the unusual case of a triplet oxygen atom stabilized by a relatively weak interaction by the Lewis acidic BeF2. The interaction involves both a donor component from oxygen to empty Be orbitals and a back-bonding contribution from fluorine substituents toward oxygen.

Transitions between triplet Rydberg states of the alkaline-earth-metal atoms for precision measurements of microwave fields

We calculated the frequencies and amplitudes of the microwave (µw) dipole transitions between triplet Rydberg states of n3S1, n3P1, n3D2, and n3F3 series in the alkaline-earth atoms. Numerical values of the amplitudes determine the µw electric-field-dependent Rabi frequency of the Rydberg level shift in the field of a resonance radiation. This shift, observed as splitting of resonance in electromagnetically induced transparency for intensely absorbed probe radiation, enables measuring the µw electric field strength. For numerical calculations, we used single-electron methods and the most reliable data on quantum defect values from the literature. We derived the asymptotic approximation formulas of the µw frequencies and amplitudes.

Theoretical Study of Ground-State Barium-Rare Gas Van der Waals Complexes: Combining Rule Modeling and Ab Initio Calculations.

The present study aims to generate the potential energy curves (PECs) and spectroscopic constants for barium alkaline earth (AE) atoms interacting with rare gas (RG) atoms (He, Ne, Ar, Kr, and Xe). The study focuses on investigating the van der Waals bonds that characterize the interactions between alkaline-earth metals and RG atoms, with a specific emphasis on employing the Tang and Toennies (TT) potential model, known to accurately describe such interactions. The TT potential model was employed in conjunction with combining rules to calculate its parameters, which include dispersion coefficients C 2n and Born-Mayer constants A and b. Additionally, we have conducted high-level ab initio calculations at the CCSD(T) level for all Ba-RG ground states. Obtained PECs from both methods have been used to evaluate the spectroscopic properties D e, R e, ωe, B e, and ωeχe. Our findings reveal that the derived spectroscopic constants from the TT model exhibit good agreement with the results obtained from CCSD(T) calculations and with other available theoretical studies. Furthermore, to gain insights into the relative differences among AE-RG species, we calculated the κ parameter for AE-RG and AE+-RG (AE = Sr, Ca, Mg, Ba; RG = He-Xe) complexes. It is found that except for the case of Ba-RG and Ba+-RG, the κ values within the same series, AE-RG and AE+-RG, are remarkably close to each other.

Quantum chemical calculations of electron affinities of alkaline earth metal atoms (Ca, Sr, Ba, and Ra)

We performed high-level ab initio quantum chemical calculations, incorporating higher-order excitations, spin–orbit coupling (SOC), and the Gaunt interaction, to calculate the electron affinities (EAs) of alkaline earth (AE) metal atoms (Ca, Sr, Ba, and Ra), which are notably small. The coupled-cluster singles and doubles with perturbative triples [CCSD(T)] method is insufficient to accurately calculate the EAs of AE metal atoms. Higher-order excitations proved crucial, with the coupled-cluster singles, doubles, and triples with perturbative quadruples [CCSDT(2)Q] method effectively capturing dynamic electron correlation effects. The contributions of SOC (ΔESOs) to the EAs calculated using the multireference configuration interaction method with the Davidson correction, including SOC, positively enhance the EAs; however, these contributions are overestimated. The Dirac–Hartree–Fock (DHF)-CCSD(T) method addresses this overestimation and provides reasonable values for ΔESO (ΔESO−D). Employing additional sets of diffuse and core–valence correlation basis sets is critical for accurately calculating the EAs of AE metal atoms. The contributions of the Gaunt interaction (ΔEGaunt) to the EAs of AE metal atoms are negligible. Notably, the CCSDT(2)Q with the complete basis set limit + ΔESO−D + ΔEGaunt produced EA values for Ca, Sr, and Ba that closely aligned with experimental data and achieved accuracy exceeding the chemical accuracy. Based on our findings, the accurately proposed EA for Ra is 9.88 kJ/mol.

Multiple Bonding in AeN- (Ae=Ca, Sr, Ba).

Quantum chemical calculations using ab initio methods at the MRCI+Q(8,9)/def2-QZVPPD and CCSD(T)/def2-QZVPPD levels as well as using density functional theory are reported for the diatomic molecules AeN- (Ae=Ca, Sr, Ba). The anions CaN- and SrN- have electronic triplet (3Π) ground states with nearly identical bond dissociation energies De ~57 kcal/mol calculated at the MRCI+Q(8,9)/def2-QZVPPD level. In contrast, the heavier homologue BaN- has a singlet (1Σ+) ground state, which is only 1.1 kcal/mol below the triplet (3Σ-) state. The computed bond dissociation energy of (1Σ+) BaN- is 68.4 kcal/mol. The calculations at the CCSD(T)-full/def2-QZVPPD and BP86-D3(BJ)/def2-QZVPPD levels are in reasonable agreement with the MRCI+Q(8,9)/def2-QZVPPD data, except for the singlet (1Σ+) state, which has a large multireference character. The calculated atomic partial charges given by the CM5, Voronoi and Hirshfeld methods suggest small to medium-sized Ae←N- charge donation for most electronic states. In contrast, the NBO method predicts for all species medium to large Ae→N- electronic charge donation, which is due to the neglect of the (n)p AOs of Ae atoms as genuine valence orbitals. Neither the bond orders nor the bond lengths correlate with the bond dissociation energies. The EDA-NOCV calculations show that the heavier alkaline earth atoms Ca, Sr, Ba use their (n)s and (n-1)d orbitals for covalent bonding.

Scalable, ab initio protocol for quantum simulating SU(N)×U(1) Lattice Gauge Theories

We propose a protocol for the scalable quantum simulation of SU(N)×U(1) lattice gauge theories with alkaline-earth like atoms in optical lattices in both one- and two-dimensional systems. The protocol exploits the combination of naturally occurring SU(N) pseudo-spin symmetry and strong inter-orbital interactions that is unique to such atomic species. A detailed ab initio study of the microscopic dynamics shows how gauge invariance emerges in an accessible parameter regime, and allows us to identify the main challenges in the simulation of such theories. We provide quantitative results about the requirements in terms of experimental stability in relation to observing gauge invariant dynamics, a key element for a deeper analysis on the functioning of such class of theories in both quantum simulators and computers.

Long-Lived Circular Rydberg Qubits of Alkaline-Earth Atoms in Optical Tweezers

Coherence time and gate fidelities in Rydberg atom quantum simulators and computers are fundamentally limited by the Rydberg state lifetime. Circular Rydberg states are highly promising candidates to overcome this limitation by orders of magnitude, as they can be effectively protected from decay due to their maximum angular momentum. We report the first realization of alkaline-earth circular Rydberg atoms trapped in optical tweezers, which provide unique and novel control possibilities due to the optically active ionic core. Specifically, we demonstrate creation of very high-n (n=79) circular states of Sr88. We measure lifetimes as long as 2.55 ms at room temperature, which are achieved via cavity-assisted suppression of black-body radiation. We show coherent control of a microwave qubit encoded in circular states of nearby manifolds, and characterize the qubit coherence time via Ramsey and spin-echo spectroscopy. Finally, circular-state tweezer trapping exploiting the Sr+ core polarizability is quantified via measurements of the trap-induced light shift on the qubit. Our work opens routes for quantum simulations with circular Rydberg states of divalent atoms, exploiting the emergent toolbox associated with the optically active core ion. Published by the American Physical Society 2024

Metal to semiconductor switching in the AgTe monolayer via decoration with alkali metal and alkaline earth metal atoms: a first-principles perspective.

In this work, employing first-principles calculations, we systematically investigate the atomic structure and electronic and optical properties of the AgTe monolayer, as well as the impact of alkali metal (Li, Na, K) and alkaline earth metal (Be, Mg, Ca) atoms decoration. The AgTe monolayer exhibits metallic characteristics. When Li, Na, K, and Mg atoms are decorated on the AgTe monolayer, the decorated AgTe monolayers are dynamically stable. In contrast, with Be and Ca atoms, the decorated structures are found to be dynamically unstable. Interestingly, the decoration of Li, Na, and K atoms into the AgTe monolayer can open the band gaps in the decorated Li-, Na- and K-AgTe monolayers around the Fermi level, leading to the actualization of metal-to-semiconductor transitions. In contrast, the decorated Mg-AgTe monolayer maintains its metallic characteristic. The highest electron and hole mobilities are achieved in the Na-AgTe monolayer among the decorated structures, suggesting the applicability of this structure in photovoltaic applications. The optical study shows that Li-, Na- and K-decorated AgTe monolayers have improved light absorption in the visible light region. Consequently, our findings shed light on the decoration of these 2D material monolayers and can potentially enhance and motivate studies in producing these monolayers for current nanodevices and future applications.

Wide band gap selenide infrared nonlinear optical materials AIIMg6Ga6Se16 with strong SHG responses and high laser-induced damage thresholds.

Infrared (IR) nonlinear optical (NLO) materials with strong NLO response, wide band gap and high laser-induced damage threshold (LIDT) are highly expected in current laser technologies. Herein, by introducing double alkaline-earth metal (AEM) atoms, three wide band gap selenide IR NLO materials AIIMg6Ga6Se16 (AII = Ca, Sr, Ba) with excellent linear and NLO optical properties have been rationally designed and fabricated. AIIMg6Ga6Se16 (AII = Ca, Sr, Ba) are composed of unique [AIISe6] triangular prisms, [MgSe6] octahedra and [GaSe4] tetrahedra. The introduction of double AEMs effectively broadens the band gaps of selenide-based IR NLO materials. Among them, CaMg6Ga6Se16, achieving the best balance between the second-harmonic generation response (∼1.5 × AgGaS2), wide band gap (2.71 eV), high LIDT (∼9 × AgGaS2), and moderate birefringence of 0.052 @ 1064 nm, is a promising NLO candidate for high power IR laser. Theoretical calculations indicate that the NLO responses and band gaps among the three compounds are mainly determined by the NLO-active [GaSe4] units. The results enrich the chemical diversity of chalcogenides, and give some insight into the design of new functional materials based on the rare [AIISe6] prismatic units.

Alkaline earth metal Atom-Doped Aza-Single-Strand pyridine Helix M@SP-Helix (M = Be, Mg, and Ca) as high-performance candidates for Single-Molecular redox SPDT NLO molecular switches

Redox molecular switch is undoubted to be a good choice for the requirement of terminal molecular device. By doping an alkaline earth metal atom into the aza-single-strand pyridine helical ligand to form M@SP-Helix (M = Be, Mg, and Ca), the alkaline earth metal atom not only act the role of providing two electrons but also the type of them can significantly affect the distribution region of every two electrons on SP-Helix in the in the redox process. Our results found that the electronic and vibrational static first hyperpolarizabilities as well as the frequency-dependent first hyperpolarizability exhibit high-performance single-pole double-throw (SPDT) nonlinear optics (NLO) switching effects from its oxidized state (off form) to neutral (on form) and to reduced states (on form) as obtaining four electrons by twice. Notably, the electronic first hyperpolarizability is increased approximately 1003- and 1.34 × 106-fold from 35 to 3.51 × 104 and 4.69 × 107 au for Ca@SP-Helix. Therefore, this work can provide a theoretical reference that the alkaline earth atom doping is an important method to design high-performance NLO molecular switch material.

State-Insensitive Trapping of Alkaline-Earth Atoms in a Nanofiber-Based Optical Dipole Trap

State-Insensitive Trapping of Alkaline-Earth Atoms in a Nanofiber-Based Optical Dipole Trap

Precision Spectroscopy of Rydberg States in Alkaline Earth Atoms for Millimeter-Wave Radiation Measurement

Precision Spectroscopy of Rydberg States in Alkaline Earth Atoms for Millimeter-Wave Radiation Measurement

A DFT study on the promising hydrogen storage performance of a light metal atom-decorated ZnO monolayer

The potential H2 adsorption/storage performance of the ZnO monolayer decorated with alkaline or alkaline earth metal atoms was studied using first-principle density functional theory (DFT) calculations. The light metal atom (Li, Na, K, Be, Mg, or Ca) could be atomically dispersed and decorated on the Zn–O hexatomic ring in the ZnO monolayer with high binding energy. Compared to Na-, K-, Be-, Mg-, or Ca-decorated ZnO, Li-decorated ZnO exhibited significantly stronger interactions with H2, resulting in higher adsorption energy, more transferred charges, and stronger orbital hybridizations. On the ZnO decorated with a single Li atom, four H2 molecules could be stored with an average adsorption energy of −0.242 eV. By increasing the two-sided Li coverage to one, three H2 molecules could still be stored on each decorated Li due to space limitations, with an acceptable average adsorption energy of −0.216 eV. As a result, the hydrogen storage capacity of the Li-decorated ZnO monolayer could be successfully and reasonably improved to 6.92 wt%. This study suggests that fully lithiated ZnO may have promising potential as an adsorbent for outstanding hydrogen storage performance.

Band topology and phase stability of half-Heusler semiconductors with d0 alkaline earth atoms

In the previous studies, the topological insulators in the half-Heusler ternary structure are assumed to be in the γ-phase having the transition metal atom at the unique middle site. In contrast, the minimum-energy half-Heusler phase can well be the β-phase with the highly electronegative anion positioned in between the electropositive metallic ions. For this subtle reason in the following a systematic study of the phase stability and the band topology of XAuZ compounds containing d0 alkaline earth atoms (X = Ca, Sr, Ba; Z = As, Sb) in their respective minimum-energy half-Heusler phases is presented. It is thus found that all the above compounds are mechanically (or dynamically) stable and have formation energies that are within a reasonable distance from the thermodynamic hull. The band structures of all compounds obtained from the more accurate TB-mBJ exchange potential with the SOC included indicate a strong band inversion such that the s-like Γ6 band falls below the p-like (Γ7+Γ8) bands. Furthermore, due to the negative spin–orbit splitting in the β-phase compounds SrAuAs and BaAuAs, the Γ8 falls below the Γ7, which opens a significant bulk insulating gap at the Fermi level. The outputs of WannierTools, such as the Z2 topological quantum numbers, surface states spectra and surface Fermi loops, indicate that the β-phase compounds SrAuAs and BaAuAs are indeed strong topological insulators with a polar character due to the lack of inversion symmetry, while non-uniform strains are needed to turn the γ-phase compounds into Weyl semimetals (ca>1) and topological insulators (ca<1).

Many-body correlations in one-dimensional optical lattices with alkaline-earth(-like) atoms

We explore the rich nature of correlations in the ground state of ultracold atoms trapped in state-dependent optical lattices. In particular, we consider interacting fermionic ytterbium or strontium atoms, realizing a two-orbital Hubbard model with two spin components. We analyze the model in one-dimensional setting with the experimentally relevant hierarchy of tunneling and interaction amplitudes by means of exact diagonalization and matrix product states approaches, and study the correlation functions in density, spin, and orbital sectors as functions of variable densities of atoms in the ground and metastable excited states. We show that in certain ranges of densities these atomic systems demonstrate strong density-wave, ferro- and antiferromagnetic, as well as antiferroorbital correlations.

Ab Initio Derivation of Lattice-Gauge-Theory Dynamics for Cold Gases in Optical Lattices

We introduce a method for quantum simulation of U$(1)$ lattice gauge theories coupled to matter, utilizing alkaline-earth(-like) atoms in state-dependent optical lattices. The proposal enables the study of both gauge and fermionic-matter fields without integrating out one of them in one and two dimensions. We focus on a realistic and robust implementation that utilizes the long-lived metastable clock state available in alkaline-earth(-like) atomic species. Starting from an $ab\,initio$ modelling of the experimental setting, we systematically carry out a derivation of the target U$(1)$ gauge theory. This approach allows us to identify and address conceptual and practical challenges for the implementation of lattice gauge theories that - while pivotal for a successful implementation - have never been rigorously addressed in the literature: those include the specific engineering of lattice potentials to achieve the desired structure of Wannier functions, and the subtleties involved in realizing the proper separation of energy scales to enable gauge-invariant dynamics. We discuss realistic experiments that can be carried out within such a platform using the fermionic isotope $^{173}$Yb, addressing via simulations all key sources of imperfections, and provide concrete parameter estimates for relevant energy scales in both one- and two-dimensional settings.