Itinerant Electrons Research Articles

Unsupervised learning of effective quantum impurity models

Generalized quantum impurity models—which feature a few localized and strongly correlated degrees of freedom coupled to itinerant conduction electrons—describe diverse physical systems, from magnetic moments in metals to nanoelectronics quantum devices such as quantum dots or single-molecule transistors. Correlated materials can also be understood as self-consistent impurity models through dynamical mean-field theory. Accurate simulation of such models is challenging, especially at low temperatures, due to many-body effects from electronic interactions, resulting in strong renormalization. In particular, the interplay between local impurity complexity and Kondo physics is highly nontrivial. A common approach, which we further develop in this work, is to consider instead a simpler effective impurity model that still captures the low-energy physics of interest. The mapping from a bare to an effective model is typically done perturbatively, but even this can be difficult for complex systems, and the resulting effective model parameters can nevertheless be quite inaccurate. Here we develop a nonperturbative, unsupervised machine learning approach to systematically obtain low-energy effective impurity-type models, based on the renormalization-group framework. The method is shown to be general and flexible, as well as accurate and systematically improvable. We benchmark the method against exact results for the Anderson impurity model, and we provide an outlook for more complex models beyond the reach of existing methods. Published by the American Physical Society 2024

Strained van der Waals Metallic Magnet for Photomagnetic Modulation and Spin Photodiode Application

AbstractAll‐optical magnetization reversal provides a low‐power approach for investigating spin state manipulation in 2D magnets. However, the ambient observation of photomagnetic coupling presents significant challenges due to the low Curie temperatures exhibited by most 2D magnets. Herein, a mixed‐dimensional heterostructure comprising a surface‐oxidized Fe3GeTe2 nanosheet with enhanced magnetic properties and individual semiconducting ZnO nanorod is proposed to explore proximity photomagnetic modulation and spin‐enhanced photodetection behaviors. The surface curvature of ZnO nanorod induces pronounced strains for Fe3GeTe2 nanosheet, leading to its anomalous Raman polarization and spin ordering at room temperature. Strain‐activated itinerant spin electrons are immobilized on the O‐2p orbitals of adjacent ZnO, thereby facilitating the optical demagnetization process in Fe3GeTe2 without aid of magnetic field. First‐principles calculations together with in situ characterization experiments further confirm that the primary charge transfer channel involves coupling between Fe3+ and oxygen vacancy defects anchored at heterointerfaces. The rapid establishment of magnetization by illumination in ZnO nanorod contributes to spin‐tunneling‐enhanced photocurrent, device response dynamics, polarization detection and ultraviolet imaging capability. These findings offer valuable insights to optimize the optoelectronic properties of conventional semiconductors and advance complex dimensional spin‐optoelectronic devices.

Solvable models of two-level systems coupled to itinerant electrons: Robust non-Fermi liquid and quantum critical pairing

Solvable models of two-level systems coupled to itinerant electrons: Robust non-Fermi liquid and quantum critical pairing

Evolution of ferromagnetism and electrical resistivity in Sb-doped Cr4PtGa17

We describe the doping effects on a metallic breathing pyrochlore compound, Cr4PtGa17. Upon doping with Sb, i.e., Cr4Pt(Ga1-xSbx)17, it was found that a selective doping on one of the seven Ga sites occurs. With increasing dopant level, the ferromagnetism in the parent compound is gradually suppressed, along with a decrease in fitted Curie-Weiss temperature (from 61 (1) K to −1.8 (1) K) and effective moment (from ∼2.26 μB/f.u. to ∼0.68 μB/f.u.). Low-temperature heat capacity measurements confirm the absence of magnetic ordering above 0.4 K for the three most doped samples. Meanwhile, electrical resistivity measurements display a metal-semiconductor transition with increasing Sb contents, which is attributed to an increase of Fermi energy based on the calculations of electronic band structure and density of states. Moreover, we have speculated that the ferromagnetism in Cr4PtGa17 is governed by itinerant electrons according to our observations. This study of Sb-doping effect on Cr4PtGa17 provides deeper understanding of magnetism of this system and possibilities for future modifications.

Unraveling the electronic structure and magnetic transition evolution across monolayer, bilayer, and multilayer ferromagnetic Fe3GeTe2

Two-dimensional (2D) van der Waals (vdW) magnets have sparked widespread attention due to their potential in spintronic applications as well as in fundamental physics. Ferromagnetic vdW compound Fe3GeTe2 (FGT) and its Ga variants have garnered significant interest due to their itinerant magnetism, correlated states, and high magnetic transition temperature. Experimental studies have demonstrated the tunability of FGT’s Curie temperature, TC, through adjustments in quintuple layer numbers (QL) and carrier concentrations, n. However, the underlying mechanism remains elusive. In this study, we employ molecular beam epitaxy (MBE) to synthesize 2D FGT films down to 1 QL with precise layer control, facilitating an exploration of the band structure and the evolution of itinerant carrier density. Angle-resolved photoemission spectroscopy (ARPES) reveals significant band structure changes at the ultra-thin limit, while first-principles calculations elucidate the band evolution from 1 QL to bulk, largely governed by interlayer coupling. Additionally, we find that n is intrinsically linked to the number of QL and temperature, with a critical value triggering the magnetic phase transition. Our findings underscore the pivotal role of band structure and itinerant electrons in governing magnetic phase transitions in such 2D vdW magnetic materials.

Tube-like Gold Clusters M2@Au17 q (M = W, Mo; q = 0, ±1): Structure, Electronic Property, and Optical Nonlinearity.

Density functional theory (DFT) calculations are carried out to determine the geometries and electronic and nonlinear optical (NLO) properties of the doubly doped gold clusters in three charge states M2 @ Au17 q with M = W, Mo and q = 0, ±1. At their lowest-lying equilibrium structures, the impurities that are vertically encapsulated inside a cylindrical gold framework, significantly enhance the stability and modify properties of the host. The presence of M2 units results in the formation of a tube-like ground state, which is identified for the first time for gold clusters. Having 30 itinerant electrons, the electron shell of M2@Au17 - can be described as 1S21P61D102S2{1F xz 2 21F yz 2 2}1F z 3 2{1F xyz 21F z(x 2-y 2) 2}{1F y(3x 2 -y 2),1F x(x 2 -3y 2)}. The species is thus stabilized upon doping, but it is not a magic cluster. The optical transitions are shifted to the lower-energy region upon doping Mo and W atoms into Au17 q . The static and dynamic NLO properties of M2@Au17 q are also computed and compared to those of the pure Au19 q (having the same number of atoms) and an external reference molecule, i.e., para-nitroaniline (p-NA). For hyperpolarizabilities, the doped clusters possess smaller values than those of their pure counterparts but much larger values than the p-NA. Of the doubly doped systems, the neutral M2@Au17 exhibits particularly high first and second hyperpolarizability tensors. The doped cluster units can also be used as building blocks for the design of gold-based nanowires with outstanding electronic and optical characteristics.

Exotic phases induced by RKKY interaction in the square lattice

We study a model of Ising spins in which direct exchange interactions compete with the Ruderman-Kittel-Kasuya-Yosida (RKKY) coupling, which may arise effectively from itinerant electrons. We consider the model in the two-dimensional square lattice and focus on values of the RKKY coupling constant (JRKKY) and the Fermi momentum (kF) that induce strong frustration. We study the low-temperature magnetic field phase diagram using Monte Carlo simulations, considering several nearest neighbors in the RKKY interaction. Magnetic frustration yields a rich phase diagram with a variety of exotic phases. We compute the structure factors and define appropriate order parameters to describe the transitions. We also discuss the validity of the approximation made for long-range couplings and analytically demonstrate the change in the coexistence lines in the phase diagram by including up to the tenth nearest neighbors.

Unusual Magnetocaloric Effect Triggered by Spin Reorientation

AbstractAdvancements and utilization of magnetic refrigeration technology hinge on the ongoing enhancement and optimization of magnetic refrigeration material properties. Nevertheless, the intricacy of the magnetocaloric effect (MCE) mechanism has emerged as a bottleneck, constraining the progress and refinement of magnetic refrigeration materials. In this study, a classic magnetic system is chosen to investigate the mechanism of MCE across four different scales–macroscopic magnetism, micrometer‐scale magnetic domains, atomic magnetic moments, and electronic structure. It simultaneously exhibits two inverse MCEs and one direct MCE, with a working temperature span as wide as 125 K (most are <50 K) for the direct MCE. The measurements of the vibrating sample magnetometer, in situ Lorentz electron microscopy and variable‐temperature neutron powder diffraction directly reveal that the complex magnetic entropy changes arise from the magnetic domain wall pinning, the instability of Ho magnetic moments, and the spin rotation. First‐principles calculations elucidate the crucial role of strong hybridization between localized Ho and itinerant Co electrons in the spin reorientation of HoCo4Al. This study contributes significantly to comprehending the induction mechanism of the MCE and holds vital reference value for exploring new magnetic refrigeration materials and enhancing MCE performance.

Point-defect modulation of hydrogen migration in Pd−based membranes

Pure hydrogen is not only one of the key ingredients in chemistry industries, but also the future fuel sources for proton-exchange membrane fuel cells and especially controlled fusion reactors. Pd and Pd−based membranes are the only commercial products for H separation and purification, which are influenced by various point defects, including vacancies and substitutional atoms. In this work, the design rationale for H diffusion process in Pd−based membranes is elucidated by intentionally modulating the electronic interaction between vacancy and H. Adding (removing) one itinerant electron in the Pd-Vacancy system strengthens (weakens) the directional bonding between H and Pd, thus facilitating (impeding) H diffusion in Pd. Extra condition is supplemented to the Hume-Rothery rules for the design of solid-solution Pd−based membranes for faster H diffusion, that is a lower-electronegativity (χ) element accelerates H diffusion by providing extra bonding electrons, while a higher one has opposite effect. Solute elements Ag (χ = 1.93), Ir (2.20), and W (2.36) in Pd (2.20) are chosen to demonstrate our design principle in real Pd-based membranes. The good agreement between experimental and theoretical results confirms the effectiveness and soundness of this new rationale, and also sheds insights into the physical picture of the complex interaction between point defects.

Metamagnetism of Itinerant Electrons in the Hubbard Model for the FCC Lattice, Caused by the Van Hove Singularity

Metamagnetism of Itinerant Electrons in the Hubbard Model for the FCC Lattice, Caused by the Van Hove Singularity

Nematic Ising superconductivity with hidden magnetism in few-layer 6R-TaS2

In van der Waals heterostructures (vdWHs), the manipulation of interlayer stacking/coupling allows for the construction of customizable quantum systems exhibiting exotic physics. An illustrative example is the diverse range of states of matter achieved through varying the proximity coupling between two-dimensional (2D) quantum spin liquid (QSL) and superconductors within the TaS2 family. This study presents a demonstration of the intertwined physics of spontaneous rotational symmetry breaking, hidden magnetism, and Ising superconductivity (SC) in the three-fold rotationally symmetric, non-magnetic natural vdWHs 6R-TaS2. A distinctive phase emerges in 6R-TaS2 below a characteristic temperature (T*) of approximately 30 K, which is characterized by a remarkable set of features, including a giant extrinsic anomalous Hall effect (AHE), Kondo screening, magnetic field-tunable thermal hysteresis, and nematic magneto-resistance. At lower temperatures, a coexistence of nematicity and Kondo screening with Ising superconductivity is observed, providing compelling evidence of hidden magnetism within a superconductor. This research not only sheds light on unexpected emergent physics resulting from the coupling of itinerant electrons and localized/correlated electrons in natural vdWHs but also emphasizes the potential for tailoring exotic quantum states through the manipulation of interlayer interactions.

Boosting spatial and energy resolution in STM with a double-functionalized probe.

The scattering of superconducting pairs by magnetic impurities on a superconducting surface leads to pairs of sharp in-gap resonances known as Yu-Shiba-Rusinov (YSR) bound states. Similar to the interference of itinerant electrons scattered by defects in normal metals, these resonances reveal a periodic texture around the magnetic impurity. The wavelength of these resonances is, however, often too short to be resolved even by methods capable of atomic resolution, i.e., scanning tunneling microscopy (STM). We combine a CO molecule with a superconducting cluster pre-attached to an STM tip to maximize both spatial and energy resolution, thus demonstrating the superior properties of such double-functionalized probes by imaging the spatial distribution of YSR states. Our approach reveals rich interference patterns of the hybridized YSR states of two Fe atoms on Nb(110), previously inaccessible with conventional STM probes. This advancement extends the capabilities of STM techniques, providing insights into superconducting phenomena at the atomic scale.

Magnetization without spin: Effective Lagrangian of itinerant electrons

In this paper, an effective Lagrangian of an itinerant electron system of finite density at a finite magnetic field is obtained. It includes a Chern-Simons term of electromagnetic potentials of lower-scale dimensions compared to those studied before. This term has an origin in the many-body wave function and a unique topological property that is independent of a spin degree of freedom. The coupling strength is proportional to ρeB, which is singular at B=0 for a constant charge density. The effective Lagrangian at a finite B represents the physical effects at B≠0 properly. A universal shift of the magnetic field known as the Slater-Pauling curve is obtained from the effective Lagrangian.

Interfacial engineering of orbital orientation for perpendicular magnetic anisotropy in Co-implanted CrI3 monolayer

Two-dimensional (2D) van der Waals (vdW) magnets are believed to be promising candidates for next-generation information storage, which requires both high Curie points (TC) and large perpendicular magnetic anisotropy (PMA). As one of the most well-known 2D magnets, CrI3 has large PMA but a relatively low TC. Recent theoretical works proposed that implanting metal atoms into the hollow sites of CrI3 could greatly boost TC. However, this process may have the unintended consequence of reducing the PMA and introducing in-plane magnetic anisotropy (IMA) instead. It is, therefore, highly required to implement an additional technique to enhance the PMA. In this work, we use the first-principles method to study the underlying mechanisms of the suppressed PMA (and induced IMA) in the Co-implanted CrI3 monolayer [denoted as Co-(CrI3)2] as an example. It is found that the Co-implantation-induced itinerant electrons cause the transition from PMA to IMA by tuning the orbital orientation of the states around the Fermi level, noting that an in-plane (or out-of-plane) electronic orbital leads to the out-of-plane (or in-plane) momentum that favors PMA (or IMA) due to the spin–orbit coupling. In order to restore the PMA, we predict that using the vdW substrate PtTe2 to construct a heterostructure with the Co-(CrI3)2 monolayer not only reduces the contributions of the interfacial out-of-plane orbitals but also generates additional intralayer in-plane orbitals, both supporting the PMA. Thus, this work provides alternative perspectives on enhancing PMA by interfacial engineering of orbital orientation, paving the way for the development of 2D strong magnets.

Odd-frequency superfluidity from a particle-number-conserving perspective

We investigate odd-in-time—or —pairing of fermions in equilibrium systems within the particle-number-conserving framework of Penrose, Onsager, and Yang, where superfluid order is defined by macroscopic eigenvalues of reduced density matrices. We show that odd-frequency pair correlations are synonymous with even fermion-exchange symmetry in a time-dependent correlation function that generalises the two-body reduced density matrix. Macroscopic even-under-fermion-exchange pairing is found to emerge from conventional Penrose-Onsager-Yang condensation in two-body or higher-order reduced density matrices through the symmetry-mixing properties of the Hamiltonian. We identify and characterize a matrix responsible for producing macroscopic even fermion-exchange correlations that coexist with a conventional Cooper-pair condensate, while a matrix is shown to be responsible for creating macroscopic even fermion-exchange correlations from hidden orders such as a multiparticle condensate. The transformer scenario is illustrated using the spin-balanced s-wave superfluid with Zeeman splitting as an example. The generator scenario is demonstrated by the composite-boson condensate arising for itinerant electrons coupled to magnetic excitations. Structural analysis of the transformer and generator matrices is shown to provide general conditions for odd-frequency pairing order to arise in a given system. Our formalism facilitates a fully general derivation of the Meissner effect for odd-frequency superconductors that holds also beyond the regime of validity for mean-field theory. Published by the American Physical Society 2024

Magnon Confinement on the Two-Dimensional Penrose Lattice: Perpendicular-Space Analysis of the Dynamic Structure Factor

Employing the spin-wave formalism within and beyond the harmonic-oscillator approx-imation, we study the dynamic structure factors of spin-12 nearest-neighbor quantum Heisenberg antiferromagnets on two-dimensional quasiperiodic lattices with particular emphasis on a mag-netic analog to the well-known confined states of a hopping Hamiltonian for independent electrons on a two-dimensional Penrose lattice. We present comprehensive calculations on the C5v Penrose tiling in comparison with the C8v Ammann–Beenker tiling, revealing their decagonal and octagonal antiferromagnetic microstructures. Their dynamic spin structure factors both exhibit linear soft modes emergent at magnetic Bragg wavevectors and have nearly or fairly flat scattering bands, signifying magnetic excitations localized in some way, at several different energies in a self-similar manner. In particular, the lowest-lying highly flat mode is distinctive of the Penrose lattice, which is mediated by its unique antiferromagnons confined within tricoordinated sites only, unlike their itinerant electron counterparts involving pentacoordinated, as well as tricoordinated, sites. Bringing harmonic antiferromagnons into higher-order quantum interaction splits, the lowest-lying nearly flat scattering band in two, each mediated by further confined antiferromagnons, which is fully demonstrated and throughly visualized in the perpendicular as well as real spaces. We disclose superconfined antiferromagnons on the two-dimensional Penrose lattice.

Antiferromagnetic Chern insulator with large charge gap in heavy transition-metal compounds

Despite the discovery of multiple intrinsic magnetic topological insulators in recent years the observation of Chern insulators is still restricted to very low temperatures due to the negligible charge gaps. Here, we uncover the potential of heavy transition-metal compounds for realizing a collinear antiferromagnetic Chern insulator (AFCI) with a charge gap as large as 300 meV. Our analysis relies on the Kane-Mele-Kondo model with a ferromagnetic Hund coupling JH\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$J_{{\ extrm{H}}}$$\\end{document} between the spins of itinerant electrons and the localized spins of size S. We show that a spin-orbit coupling λSO≳0.03t\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\lambda _{{\ extrm{SO}}} \\gtrsim 0.03t$$\\end{document}, where t is the nearest-neighbor hopping element, is already large enough to stabilize an AFCI provided the alternating sublattice potential δ\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\delta$$\\end{document} is in the range δ≈SJH\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\delta \\approx SJ_{{\ extrm{H}}}$$\\end{document}. We establish a remarkable increase in the charge gap upon increasing λSO\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\lambda _{{\ extrm{SO}}}$$\\end{document} in the AFCI phase. Using our results we explain the collinear AFCI recently found in monolayers of CrO and MoO with charge gaps of 1 and 50meV\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$50\\,\\hbox {meV}$$\\end{document}, respectively. In addition, we propose bilayers of heavy transition-metal oxides of perovskite structure as candidates to realize a room-temperature AFCI if grown along the [111] direction and subjected to a perpendicular electric field.

Spin-Charge-Lattice Coupling across the Charge Density Wave Transition in a Kagome Lattice Antiferromagnet.

Understanding spin and lattice excitations in a metallic magnetic ordered system forms the basis to unveil the magnetic and lattice exchange couplings and their interactions with itinerant electrons. Kagome lattice antiferromagnet FeGe is interesting because it displays a rare charge density wave (CDW) deep inside the antiferromagnetic ordered phase that interacts with the magnetic order. We use neutron scattering to study the evolution of spin and lattice excitations across the CDW transition T_{CDW} in FeGe. While spin excitations below ∼100 meV can be well described by spin waves of a spin-1 Heisenberg Hamiltonian, spin excitations at higher energies are centered around the Brillouin zone boundary and extend up to ∼180 meV consistent with quasiparticle excitations across spin-polarized electron-hole Fermi surfaces. Furthermore, c-axis spin wave dispersion and Fe-Ge optical phonon modes show a clear hardening below T_{CDW} due to spin-charge-lattice coupling but with no evidence of a phonon Kohn anomaly. By comparing our experimental results with density functional theory calculations in absolute units, we conclude that FeGe is a Hund's metal in the intermediate correlated regime where magnetism has contributions from both itinerant and localized electrons arising from spin polarized electronic bands near the Fermi level.

Origin of the metamagnetic transitions in Y0.9Tb0.1Fe2D4.3

Deuterium insertion was used to tune the magnetic properties of Y0.9Tb0.1Fe2 Laves phase towards an itinerant electron metamagnetic (IEM) behavior. The latter is highly sensitive to chemical changes and external parameters. The structural and magnetic properties of Y0.9Tb0.1Fe2D4.3 were investigated using various neutron powder diffraction experiments in addition to magnetic measurements under steady and pulsed high magnetic fields up to 60 T. The deuteride crystallizes in a monoclinic structure (Pc space group) with 4.3 D atoms located in 18 tetrahedral interstitial sites. At zero field, it undergoes a ferrimagnetic-antiferromagnetic (FiM-AFM) transition at TM0 = 90 K, accompanied by an anisotropic magnetostriction and a negative cell volume expansion of 0.6 %. A second AFM-PM transition is observed at 146 K. Under pulsed magnetic field at 4.2 K, the deuteride displays a multistep magnetic behavior from ferrimagnetic to a ferromagnetic state, which can be attributed to a stepwise rotation of the Tb moments. The ZFC-FC magnetization curves at low fields exhibit an irreversibility below 90 K, followed by a sharp decrease in magnetization at the FM-AFM transition. Between 90 K and 130 K, the magnetization curves display an IEM behavior, with the transition field increasing linearly with temperature.

Revealing a distortive polar order buried in the Fermi sea.

Polar metals are challenging to identify spectroscopically because the fingerprints of electric polarization are often obscured by the presence of screening charges. Here, we unravel unambiguous signatures of a distortive polar order buried in the Fermi sea by probing the nonlinear optical response of materials driven by tailored terahertz fields. We apply this strategy to investigate the topological crystalline insulator Pb1-xSnxTe, tracking its soft phonon mode in the time domain and observing the occurrence of inversion symmetry breaking as a function of temperature. By combining measurements across the material's phase diagram with ab initio calculations, we demonstrate the generality of our approach. These results highlight the potential of terahertz driving fields to reveal polar orders coexisting with itinerant electrons, thus opening additional avenues for material discovery.