Gauge invariance from on-shell massive amplitudes and tree-level unitarity
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79 ASTRONOMY AND ASTROPHYSICS↗
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Electrical Control of the Nuclear Spin States of Rare-Earth Adatoms
Rare-earth adatoms on surfaces have been studied for potential atomic-scale magnetic storage, quantum sensing, and quantum computing applications. Despite accumulating experimental efforts, a comprehensive description of the electronic configurations of the adatoms remains elusive. Here, we investigate two charge states and several electronic configurations, including 5d and 6s valence shells, for a Sm adatom on a MgO substrate using multiconfigurational ab initio methods, for the possibility of using the Sm nuclear spin levels as qubits. For the configurations in a neutral charge state, we find that the electronic ground state is a singlet, and thus the hyperfine interaction associated with the 147 Sm nucleus is absent, which may greatly enhance nuclear spin coherence time. The degeneracy of the nuclear levels is lifted by the nuclear quadrupole interaction. We show that the splitting of the nuclear levels can be controlled by a static electric field, and that Rabi oscillations between the nuclear levels can be induced by a time-dependent electric field. For the configurations in a singly charged state, electronic Kramers doublets are formed. The electronic configurations including an unpaired 6s orbital exhibit a strong hyperfine Stark effect due to a large Fermi contact contribution to the hyperfine interaction. In these configurations, electric-field-induced Rabi oscillations between the electronic-nuclear levels can occur at frequencies up to 3 orders of magnitude higher than those for the neutral charge state. The proposed system may be experimentally observed within scanning tunneling microscopy.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Synthesis of PbS/CdS/Cu 2-x S core/shell/shell quantum dots for rapid NIR emission.
Nanoscale semiconductors, known as quantum dots (QDs), possess unique size-tunable optical and electrical properties. With continued research into quantum information storage and quantum communication, the need for near-infrared single photon emitters and absorbers has gained prominence. Lead sulfide QDs have only recently been explored as a reliable near-infrared single photon emitters with the addition of a protective cadmium sulfide shell. Despite the increased air and room temperature stability of these QDs, long photon emission times have limited widespread application. This work examines the enhanced photon emission due to the Purcell effect provided by the layering of copper sulfide. In particle, this work synthesized lead sulfide cores in the 10 nm range, successfully layered cadmium sulfide through cation exchange, and attempted the cation exchange of copper sulfide, as identified with near-infrared absorbance spectra, transmission electron microscopy, and photoluminescence spectra.
36 MATERIALS SCIENCE↗
Spin-free formulation of the multireference driven similarity renormalization group: A benchmark study of first-row diatomic molecules and spin-crossover energetics
We report a spin-free formulation of the multireference (MR) driven similarity renormalization group (DSRG) based on the ensemble normal ordering of Mukherjee and Kutzelnigg (1997). This ensemble averages over all microstates of a given total spin quantum number, and therefore, it is invariant with respect to SU(2) transformations. As such, all equations may be reformulated in terms of spin-free quantities and they closely resemble those of spin-adapted closed-shell coupled cluster (CC) theory. The current implementation is used to assess the accuracy of various truncated MR-DSRG methods (perturbation theory up to third order and iterative methods with single and double excitations) in computing the constants of 33 first-row diatomic molecules. The accuracy trends for these first-row diatomics are consistent with our previous benchmark on a small subset of closed-shell diatomic molecules. We then present the first MR-DSRG application on transition-metal complexes by computing the spin splittings of the [Fe(H 2 O) 6 ] 2+ and [Fe(NH 3 ) 6 ] 2+ molecules. A focal point analysis (FPA) shows that third-order perturbative corrections are essential to achieve reasonably converged energetics. The FPA based on the linearized MR-DSRG theory with one- and two-body operators and up to a quintuple- ζ basis set predicts the spin splittings of [Fe(H 2 O) 6 ] 2+ and [Fe(NH 3 ) 6 ] 2+ to be –35.7 and –17.1 kcal mol –1 , respectively, showing good agreement with the results of local CC theory with singles, doubles, and perturbative triples.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Accurate and efficient description of interacting carriers in quantum nanostructures by selected configuration interaction and perturbation theory
In this paper, we present a method to accurately and efficiently calculate many-body states of interacting carriers in quantum nanostructures based on a combination of iterative selection of configurations and perturbation theory. This method enables investigations of large excitonic complexes and multielectron systems with near full configuration interaction accuracy, even though only a small subspace of the full many-body Hilbert space is sampled, thus saving orders of magnitudes in computational resources. Important advantages of this method are that the convergence is controlled by a single parameter, the threshold, and that ground and excited states can be treated on an equal footing. On the example of InAsP nanowire quantum dots described using a million-atom tight-binding approach, we demonstrate the extreme efficiency of the method by numerical studies of large excitonic complexes filling up to the fourth electronic shell. We find that the method generally converges fast as a function of the threshold, profiting from a significant acceleration due to the perturbative corrections. The role of the choice of single-particle basis states is discussed. It is found that the algorithm converges faster in the Hartree-Fock basis only for highly charged systems, where Coulomb repulsion dominates. Finally, based on the observation that second-order perturbative energy corrections only depend on off-diagonal elements of the many-body Hamiltonian, we present a way to accurately calculate many-body states that requires only a relatively small number of Coulomb matrix elements.
36 MATERIALS SCIENCE↗
Critical role of magnetic moments in heavy-fermion materials: Revisiting mysteries of SmB 6
Heavy-fermion family exhibits fascinating and often puzzling properties due to the presence of open-shell f ions and the complexity of the associated charge, orbital, and spin degrees of freedom. SmB 6 is a prototypical heavy-fermion compound that is electrically insulating but yet it displays quantum oscillations, which are a telltale signature of the metallic state. Adding to the enigma is the possibility that SmB 6 is a topological Kondo insulator. Here, by treating the spin degree of freedom on an equal footing with other degrees of freedom using the parameter-free strongly-constrained and appropriately-normed (SCAN) density functional, we explore the ground-state electronic structure of SmB6. A number of competing magnetic phases lying very closely in energy are found, indicating the key role of spin fluctuations in the material. The computed band structure, crystal-field splittings in the f-electron complex, the heavy effective electron mass at the Fermi energy, and the large specific heat are all in good agreement with the corresponding experimental results. In particular, our predicted FS explains the experimentally observed bulk quantum oscillations as well as the low electrical conductivity of SmB 6 . The topological Kondo state of SmB6 is shown to be robust regardless of its magnetic configuration. The excellent performance of SCAN in heavy-fermion systems is explained in terms of its ability to treat self-interaction errors and symmetry breaking within the framework of the density functional theory. Our study provides a new approach for modeling heavy-fermion materials
36 MATERIALS SCIENCE↗
Kondo effect in ferromagnetic quantum critical CeRh 6 Ge 4
The mechanism of a pressure-induced quantum critical point in the heavy fermion ferromagnet CeRh 6 Ge 4 has attracted interest, as ferromagnetic quantum criticality in a clean itinerant Ce compound is typically avoided. The localized versus itinerant character of the 4𝑓 electrons is a key aspect for understanding this behavior. We investigated the electronic structure of the 4𝑓 shell in CeRh 6 Ge 4 using core-level photoelectron and x-ray absorption spectroscopy, demonstrating the hybridization of Ce 4𝑓 with the conduction electrons. Linearly polarized x-ray absorption reveals a temperature-dependent linear dichroism consistent with the crystal-electric-field sequence as inferred from the static susceptibility. This dichroism cannot be described by an ionic full-multiplet model alone, but is reproduced by including the Kondo effect within a single-impurity Anderson model in the noncrossing approximation. The Kondo effect mixes higher-lying crystal-field states into a resulting multiorbital ground state with 4𝑓 occupancy, 𝑛 𝑓 ∼ 0.9. Deviations at low temperatures between the measured linear dichroism and calculated dichroism suggest an orbital-dependent Kondo effect. A scenario in which there is a multiorbital ground state and orbital-dependent Kondo hybridization should be a starting point for a model of pressure-induced criticality in CeRh 6 Ge 4 .
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Electronic landscape of the f -electron intermetallics with the ThCr 2 Si 2 structure
Although strongly correlated f -electron systems are well known as reservoirs for quantum phenomena, a persistent challenge is to design specific states. What is often missing are simple ways to determine whether a given compound can be expected to exhibit certain behaviors and what tuning vector(s) would be useful to select the ground state. In this review, we address this question by aggregating information about Ce, Eu, Yb, and U compounds with the ThCr 2 Si 2 structure. We construct electronic/magnetic state maps that are parameterized in terms of unit cell volumes and d -shell filling, which reveals useful trends including that (i) the magnetic and nonmagnetic examples are well separated, and (ii) the crossover regions harbor the examples with exotic states. These insights are used to propose structural/chemical regions of interest in these and related materials, with the goal of accelerating discovery of the next generation of f -electron quantum materials.
42 ENGINEERING↗
Looking at extremal black holes from very far away
Near-extremal black holes are subject to large quantum effects, which modify their low-temperature thermodynamic behavior. Hitherto, these quantum effects were analyzed by separating the geometry into the near-horizon region and its exterior. It is desirable to understand and reproduce such corrections from the full higher-dimensional asymptotically flat or AdS geometry’s perspective. We address this question in this article and fill this gap. Specifically, we find off-shell eigenmodes of the quadratic fluctuation operator of the Euclidean gravitational dynamics, with eigenvalues that vanish linearly with temperature. We illustrate this for BTZ and neutral black holes with hyperbolic horizons in AdS in Einstein-Hilbert theory, and for the charged black holes in Einstein-Maxwell theory. The linear scaling with Matsubara frequency, which is a distinctive feature of the modes, together with the fact that their wavefunctions localize close to the horizon as we approach extremality, identifies them as responsible for the aforementioned quantum effects. We provide a contour prescription to deal with the sign indefiniteness of the Euclidean Einstein-Maxwell action, which we derive to aid our analysis. We also resolve a technical puzzle regarding modes associated with rotational isometries in stationary black hole spacetimes.
AdS-CFT Correspondence↗
Fermion geometry and the renormalization of the Standard Model Effective Field Theory
The geometry of field space governs on-shell scattering amplitudes. We formulate a geometric description of effective field theories which extends previous results for scalars and gauge fields to fermions. The field-space geometry reorganizes and simplifies the computation of quantum loop corrections. Using this geometric framework, we calculate the fermion loop contributions to the renormalization group equations for bosonic operators in the Standard Model Effective Field Theory up to mass dimension eight.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Zero-Field Splitting Calculations by Multiconfiguration Pair-Density Functional Theory
Zero-field splitting (ZFS) is a fundamental molecular property that is especially relevant for single-molecule magnets (SMMs), electron paramagnetic resonance spectra, and quantum computing. Developing a method that can accurately predict ZFS parameters can be very powerful for designing new SMMs. One of the challenges is to include external correlation in an inherently multiconfigurational open-shell species for the accurate prediction of magnetic properties. Previously available methods depend on expensive multireference perturbation theory calculations to include external correlation. In this paper, we present spin-orbit-inclusive multiconfiguration and multistate pair-density functional theory (MC-PDFT) calculations of ZFSs; these calculations have a cost comparable to complete-active-space self-consistent field (CASSCF) theory, but they include correlation external to the active space. We found that combining a multistate formulation of MC-PDFT, namely, compressed-state multistate pair-density functional theory, with orbitals optimized by weighted-state-averaged CASSCF, yields reasonably accurate ZFS results
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Theoretical Examination of the Hydroxide Transport in Cobaltocenium-Containing Polyelectrolytes
Polymers incorporating cobaltocenium groups have received attention as promising components of anion-exchange membranes (AEMs), exhibiting a good balance of chemical stability and high ionic conductivity. In this work, we analyze the hydroxide diffusion in the presence of cobaltocenium cations in an aqueous environment based on the molecular dynamics of model systems confined in one dimension to mimic the AEM channels. In order to describe the proton hopping mechanism, the forces are obtained from the electronic structure computed at the density-functional tight-binding level. We find that the hydroxide diffusion depends on the channel size, modulation of the electrostatic interactions by the solvation shell, and its rearrangement ability. Hydroxide diffusion proceeds via both the vehicular and structural diffusion mechanisms with the latter playing a larger role at low diffusion coefficients. The highest diffusion coefficient is observed under moderate water densities (around half the density of liquid water) when there are enough water molecules to form the solvation shell, reducing the electrostatic interaction between ions, yet there is enough space for the water rearrangements during the proton hopping. Furthermore, the effects of cobaltocenium separation, orientation, chemical modifications, and the role of nuclear quantum effects are also discussed.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
A precision test of averaging in AdS/CFT
We reconsider the role of wormholes in the AdS/CFT correspondence. We focus on Euclidean wormholes that connect two asymptotically AdS or hyperbolic regions with $\mathbb{S}$ 1 × $\mathbb{S}$ d-1 boundary. There is no solution to Einstein’s equations of this sort, as the wormholes possess a modulus that runs to infinity. To find on-shell wormholes we must stabilize this modulus, which we can do by fixing the total energy on the two boundaries. Such a wormhole gives the saddle point approximation to a non-standard problem in quantum gravity, where we fix two asymptotic boundaries and constrain the common energy. Crucially the dual quantity does not factorize even when the bulk is dual to a single CFT, on account of the fixed energy constraint. From this quantity we extract a smeared version of the microcanonical spectral form factor. For a chaotic theory this quantity is self-averaging, i.e. well-approximated by averaging over energy windows, or over coupling constants. We go on to give a precision test involving the microcanonical spectral form factor where the two replicas have slightly different coupling constants. In chaotic theories this form factor is known to smoothly decay at a rate universally predicted in terms of one replica physics, provided that there is an average either over a window or over couplings. We compute the expected decay rate for holographic theories, and the form factor from a wormhole, and the two exactly agree for a wide range of two-derivative effective field theories in AdS. This gives a precision test of averaging in AdS/CFT. Our results interpret a number of confusing facts about wormholes and factorization in AdS and suggest that we should regard gravitational effective field theory as a mesoscopic description, analogous to semiclassical mesoscopic descriptions of quantum chaotic systems.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Multiscale Physics of Atomic Nuclei from First Principles
Atomic nuclei exhibit multiple energy scales ranging from hundreds of MeV in binding energies to fractions of an MeV for low-lying collective excitations. As the limits of nuclear binding are approached near the neutron and proton drip lines, traditional shell structure starts to melt with an onset of deformation and an emergence of coexisting shapes. It is a long-standing challenge to describe this multiscale physics starting from nuclear forces with roots in quantum chromodynamics. Here, we achieve this within a unified and nonperturbative quantum many-body framework that captures both short- and long-range correlations starting from modern nucleon-nucleon and three-nucleon forces from chiral effective field theory. The short-range (dynamic) correlations which account for the bulk of the binding energy are included within a symmetry-breaking framework, while long-range (static) correlations (and fine details about the collective structure) are included by employing symmetry projection techniques. Our calculations accurately reproduce—within theoretical error bars—available experimental data for low-lying collective states and the electromagnetic quadrupole transitions in 20−30 Ne. In addition, we reveal coexisting spherical and deformed shapes in 30 Ne, which indicates the breakdown of the magic neutron number 𝑁 = 20 as the key nucleus 28 O is approached, and we predict that the drip line nuclei 32,34 Ne are strongly deformed and collective. By developing reduced-order models for symmetry-projected states, we perform a global sensitivity analysis and find that the subleading singlet 𝑆-wave contact and a pion-nucleon coupling strongly impact nuclear deformation in chiral effective field theory. The techniques developed in this work clarify how microscopic nuclear forces generate the multiscale physics of nuclei spanning collective phenomena as well as short-range correlations and allow one to capture emergent and dynamical phenomena in finite fermion systems such as atom clusters, molecules, and atomic nuclei.
74 ATOMIC AND MOLECULAR PHYSICS↗
Symmetry Breaking in the Lowest-Lying Excited-State of CCl4: Valence Shell Spectroscopy in the 5.0–10.8 eV Photon Energy Range
We report absolute high-resolution vacuum ultraviolet (VUV) photoabsorption cross-sections of carbon tetrachloride (CCl4) in the photon energy range 5.0–10.8 eV (248–115 nm). The molecular spectrum and electronic structure have been comprehensively investigated together with quantum chemical calculations, providing geometries, bond lengths, vertical excitation energies and oscillator strengths. The major electronic excitations have been assigned to valence and Rydberg transitions which are also accompanied by vibrational excitation assigned to degenerate stretching, v3′t2 and degenerate deformation v4′t2 modes. The rather complex nuclear dynamics along the degenerate deformation mode, v4′t2, have been thoroughly investigated by Time-Dependent Density Functional Theory (TD-DFT) method. The relevant Jahn–Teller distortion operative within the lowest-lying electronic excited-state is shown here for the first time in order to yield a weak absorption feature at 6.156 eV. Further calculations on the potential energy curves for the singlet excited-states along the C–Cl stretching coordinate show the relevance of efficient C–Cl bond excision.
Biochemistry & Molecular Biology↗
Sn-InAs Nanowire Shadow-Defined Josephson Junctions
Hybrid superconductor–semiconductor platforms are foundational to advancing quantum information technologies, motivating the integration of materials with clean interfaces, robust superconductivity, and scalable architectures. Here, in this work, we report the synthesis and analysis of inclined InAs nanowires, conformally coated with β-Sn shells. These nanowires extend in opposite in-plane directions, forming a self-aligned, criss-cross network. This enables the deterministic formation of nanowire-shadow Josephson junctions through angle-controlled, low-temperature Sn deposition. Structural characterization shows uniform polycrystalline β-Sn shells forming a sharp, diffusion-free interface with InAs. Low-temperature transport measurements reveal a hard induced superconducting gap ≈ 600 μeV, switching currents up to ≈ 500 nA, and parallel magnetic field resilience beyond 1T. These results establish β-Sn/InAs nanowire networks as a promising platform for superconducting qubits, low-noise microwave devices, and the exploration of exotic superconducting phases including triplet pairing and topological superconductivity.
B-Sn↗
The O K -2 V spectrum of CO: the influence of the second core-hole
Using synchrotron radiation in the tender X-ray regime, a photoelectron spectrum showing the formation of single site double-core-hole pre-edge states, involving the K shell of the O atom in CO, has been recorded by means of high-resolution electron spectroscopy. The experimentally observed structures have been simulated, interpreted and assigned, employing state-of-the-art ab initio quantum chemical calculations, on the basis of a theoretical model, accounting for their so-called direct or conjugate character. Features appearing above the double ionization threshold have been reproduced by taking into account the strong mixing between multi-excited and continuum states. The shift of the σ* resonance below the double ionization threshold, in combination with the non-negligible contributions of multi-excited configurations in the final states reached, gives rise to a series of avoided crossings between the different potential energy curves.
74 ATOMIC AND MOLECULAR PHYSICS↗
Extremely Slow Trap-Mediated Hole Relaxation in Room-Temperature InP/ZnSe/ZnS Quantum Dots
Time-resolved photoluminescence (PL) and transient absorption (TA) spectroscopy have been used to elucidate the hole relaxation dynamics in high-quality InP/ZnSe/ZnS quantum dots (QDs) at room temperature. In QDs having an In/P ratio close to 1:1, hole cooling is fast compared to the ~40 ps time-correlated photon-counting instrument response. However, in QDs that luminesce at wavelengths greater than around 600 nm and have excess indium, a significant fraction of the PL exhibits a slower rise time. In this case, the PL rises over a range of timescales varying from close to the instrument response to approximately 300–400 ps. The time constant of the slowest component increases with increasing InP core size and the fraction of the PL that has the slow rise time increases with excess indium in the particle. In all cases, a slow rise time and any spectral evolution on that timescale are absent in the TA results, indicating that the slow dynamics may be assigned to relaxation in the valence band. QDs emitting at wavelengths below 560 nm show very different dynamics, exhibiting a barely detectable <50 ps rise time. Based on these results and measured elemental compositions, the slow hole relaxation is assigned to the transient population of indium-based traps in the ZnSe shell that are above the valence band edge only for the larger, red-emitting QDs. Here, the relative trap to band edge relaxation rates can be understood in terms of effective mass approximation hole wave function calculations, which show that the relaxation rate is largely determined by the extent to which the hole wave function in the lowest exciton penetrates into the ZnSe shell, overlapping the trapped-hole wave functions.
77 NANOSCIENCE AND NANOTECHNOLOGY↗