Electron Systems Research Articles

The Analysis of Electron Densities: From Basics to Emergent Applications.

The electron density determines all properties of a system of nuclei and electrons. It is both computable and observable. Its topology allows gaining insight into the mechanisms of bonding and other phenomena in a way that is complementary to and beyond that available from the molecular orbital picture and the formal oxidation state (FOS) formalism. The ability to derive mechanistic insight from electron density is also important with methods where orbitals are not available, such as orbital-free density functional theory (OF-DFT). While density topology-based analyses such as QTAIM (quantum theory of atoms-in-molecules) have been widely used, novel, vector-based techniques recently emerged such as next-generation (NG) QTAIM. Density-dependent quantities are also actively used in machine learning (ML)-based methods, in particular, for ML DFT functional development, including machine-learnt kinetic energy functionals. We review QTAIM and its recent extensions such as NG-QTAIM and localization-delocalization matrices (LDM) and their uses in the analysis of bonding, conformations, mechanisms of redox reactions excitations, as well as ultrafast phenomena. We review recent research showing that direct density analysis can circumvent certain pitfalls of the FOS formalism, in particular in the description of anionic redox, and of the widely used (spherically) projected density of states analysis. We discuss uses of density-based quantities for the construction of DFT functionals and prospects of applications of analyses of density topology to get mechanistic insight with OF-DFT and recently developed time-dependent OF-DFT.

Absorption of electromagnetic waves in a screened two-dimensional electron system

Absorption of electromagnetic waves in a screened two-dimensional electron system

Bulk and shear viscosities in a multicomponent two-dimensional electron system

Bulk and shear viscosities in a multicomponent two-dimensional electron system

Search for Pauli Exclusion Principle violations with Gator at LNGS

The Pauli Exclusion Principle (PEP) appears from fundamental symmetries in quantum field theories, but its physical origin is still to be understood. High-precision experimental searches for small PEP violations permit testing key assumptions of the Standard Model with high sensitivity. We report on a dedicated measurement with Gator, a low-background, high-purity germanium detector operated at the Laboratori Nazionali del Gran Sasso, aimed at testing PEP-violating atomic transitions in lead. The experimental technique, relying on forming a new symmetry state by introducing electrons into the pre-existing electron system through a direct current, satisfies the conditions of the Messiah-Greenberg superselection rule. No PEP violation has been observed, and an upper limit on the PEP violation probability of β2/2<4.8·10-29\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\beta ^2/2 < 4.8 \\cdot 10^{-29}$$\\end{document} (90% CL) is set. This improves the previous constraint from a comparable measurement by more than one order of magnitude.

Subwavelength-modulated silicon photonics for low-energy free-electron-photon interactions

We investigate silicon waveguides with subwavelength-scale modulation for applications in free-electron-photon interactions. The modulation enables velocity matching and efficient interactions between low-energy electrons and co-propagating photons. Specifically, we design a subwavelength-grating (SWG) waveguide for interactions between 23-keV free electrons and ≈1500-nm photons. The SWG waveguide and electron system exhibit a coupling coefficient of |gQu| = 0.23, and as we corroborate with time-domain, particle-in-cell simulations, the system operates as a backward-wave oscillator. Overall, our results show that modulated waveguides could open the door to strong, extended interactions between photons and low-energy (10-keV-scale) electrons, like those typically present in scanning electron microscopes. Additionally, our SWG waveguide design suggests that periodic waveguides could offer intriguing dispersion engineering opportunities for tailoring these interactions.

Dimensionally Extending from 1D MX-Chain to Ladder and Nanotube Systems: Structural and Electronic Properties.

Molecular one-dimensional (1D) electron systems have attracted much attention due to their unique electronic state, physical and chemical properties derived from high-aspect-ratio structures. Among 1D materials, mixed-valence halogen-bridged transition-metal chain complexes (MX-chains) based on coordination assemblies are currently of particular interest because their electronic properties, such as mixed-valence state and band gap, can be controlled by substituting components and varying configurations. In particular, chemistry has recently noted that dimensionally extending MX-chains through organic rung ligands can introduce and modulate electronic coupling of metal atoms between chains, i. e., interchain interactions. In this review, for the first time, we highlight the recent progress on MX systems from the viewpoint of dimensionally extending from 1D chain to ladder and nanotube, mainly involving structural design and electronic properties. Overall, dimensional extension can not only tune the electronic properties of MX-chain, but also build the unique platform for studying transport dynamics in confined space, such as proton conduction. Based on these features, we envision that the MX-chain systems provide valuable insights into deep understanding of 1D electron systems, as well as the potential applications such as nanoelectronics.

Dirac-Like Fermions Anomalous Magneto-Transport in a Spin-Polarized Oxide 2D Electron System.

In a 2D electron system (2DES) the breaking of the inversion, time-reversal and bulk crystal-field symmetries is interlaced with the effects of spin-orbit coupling (SOC) triggering exotic quantum phenomena. Here, epitaxial engineering is used to design and realize a 2DES characterized simultaneously by ferromagnetic order, large Rashba SOC and hexagonal band warping at the (111) interfaces between LaAlO3, EuTiO3, and SrTiO3 insulators. The 2DES displays anomalous quantum corrections to the magneto-conductance driven by the time-reversal-symmetry breaking occurring below the magnetic transition temperature. The results are explained by the emergence of a non-trivial Berry phase and competing weak anti-localization/weak localization back-scattering of Dirac-like fermions, mimicking the phenomenology of gapped topological insulators. These findings open perspectives for the engineering of novel spin-polarized functional 2DES holding promises in spin-orbitronics and topologicalelectronics.

Proximity-Induced Superconductivity in a 2D Kondo Lattice of an f-Electron-Based Surface Alloy.

Realizing hybrids of low-dimensional Kondo lattices and superconducting substrates leads to fascinating platforms for studying the exciting physics of strongly correlated electron systems with induced superconducting pairing. Here, we report a scanning tunneling microscopy and spectroscopy study of a new type of two-dimensional (2D) La-Ce alloy grown epitaxially on a superconducting Re(0001) substrate. We observe the characteristic spectroscopic signature of a hybridization gap evidencing the coherent spin screening in the 2D Kondo lattice realized by the ultrathin La-Ce alloy film on normal conducting Re(0001). Upon lowering the temperature below the critical temperature of rhenium, a superconducting gap is induced exhibiting an energy asymmetry of the coherence peaks that arises from the interaction of residual unscreened magnetic moments with the superconducting substrate. A positive correlation between the Kondo hybridization gap and the asymmetry of the coherence peaks is found.

Accurate Calculation of Interatomic Forces with Neural Networks Based on a Generative Transformer Architecture.

Using neural networks to express electronic wave functions represents a new paradigm for solving the Schrödinger equation in quantum chemistry. For practical quantum chemistry simulations, one needs to know not only energies of molecules, but also accurate forces acting on constituent atoms. In this work, we achieve the accurate calculation of interatomic forces on QiankunNet, a platform that combines transformer-based deep neural networks with efficient batched autoregressive sampling. Our approach permits the application of the Hellmann-Feynman theorem to force calculations without introducing corrective Pulay terms. The results show that the calculated interatomic forces are in close agreement with those derived from the full configuration interaction method, irrespective of whether the system is a simple molecule or a strongly correlated electron system like a linear hydrogen chain. Furthermore, the calculated interatomic forces are employed for atomic relaxation in the torsional rotation process of ethylene, and the energy barrier obtained from the scanned potential energy surface is in excellent agreement with the experiment. Our work contributes to the application of artificial intelligence to broader quantum chemistry simulations, such as modeling challenging chemical transformations where electron correlations are difficult to describe.

DFT study of electronic and nonlinear optical properties of alkaline earth metals and superalkalis doped all-cis-1, 2, 3, 4, 5, 6-hexafluorocyclohexane as an efficient excess electron system

Continual advancements are being pursued to discover innovative strategies for developing materials with remarkable nonlinear optical (NLO) response. Herein, electronic, geometric, thermodynamic and NLO properties of excess electron systems based on stacked Janus dimer, all-cis-1,2,3,4,5,6-hexafluorocyclohexane (C6H6F6)2 are thoroughly investigated. The excess electron systems are designed by doping alkaline earth metals (AEMs) on fluorine face and superalkalis on hydrogen face of Janus dimer. The higher values of vertical ionization energies (VIE) and interaction energies (Eint), confirm the electronic and thermodynamic stabilities of the designed complexes, respectively. Natural bond orbital (NBO) analysis is performed, and the excess electron character of the complexes is confirmed through frontier molecular orbital (FMO) analysis by highest occupied molecular orbital (HOMO) iso-densities. FMO shows a significant decrease in energy gaps (Egap) of the complexes (i.e., Eg = 1.80–3.12 eV), compared to the stacked Janus dimer (i.e., Eg = 9.41 eV). The transparency of the complexes to UV region is confirmed through UV–vis analyses, revealing their maximum absorption in visible and near-IR regions. The higher NLO response of the designed excess electron systems is further proved by the greater values of first hyperpolarizability (β o ) i.e., up to 1.70 × 106 au. Moreover, the time dependent-density functional theory (TD-DFT) computations and two-level model are employed to investigate the controlling factors of hyperpolarizability, illustrating the contribution of transition energy (∆E3), change in dipole moment (∆μ) and oscillator strength (f o ) in controlling the β o . Ab-initio molecular dynamics (AIMD) simulation further confirm that the designed superalkalide complexes are kinetically and thermally stable. The thorough investigation of these excess electron systems proves them an appropriate candidate for NLO applications.

Localizing Transitions via Interaction-Induced Flat Bands.

This Letter presents a theory of interaction-induced band-flattening in strongly correlated electron systems. We begin by illustrating an inherent connection between flat bands and index theorems, and presenting a generic prescription for constructing flat bands by periodically repeating local Hamiltonians with topological zero modes. Specifically, we demonstrate that a Dirac particle in an external, spatially periodic magnetic field can be cast in this form. We derive a condition on the field to produce perfectly flat bands and provide an exact analytical solution for the flat band wave functions. Furthermore, we explore an interacting model of Dirac fermions in a spatially inhomogeneous field. We show that certain Hubbard-Stratonovich configurations exist that "rectify" the field configuration, inducing band flattening. We present an explicit model where this localization scenario is energetically favorable-specifically in Dirac systems with nearly flat bands, where the energy cost of rectifying textures is quadratic in the order parameter, whereas the energy gain from flattening is linear. In conclusion, we discuss alternative symmetry-breaking channels, especially superconductivity, and propose that these interaction-induced band-flattening scenarios represent a generic nonperturbative mechanism for spontaneous symmetry breaking, pertinent to many strongly correlated electron systems.

The Migdal jump under the quantum Hall regime

In two-dimensional electron systems at large values of the Wigner-Seits parameter rs and in the quantum Hall effect mode, the distribution function of particles over Landau levels was calculated. It turned out that at small filling factors, the tail of the distribution function and the magnitude of the Migdal jump are qualitatively different from the case of a Fermi liquid in a zero magnetic field. Due to the presence of the cyclotron energy gap, the Fermi-liquid distortion of the distribution function is significantly suppressed.

Optical spectroscopy of an excited Laughlin liquid

Neutral excitations with zero momentum in a Laughlin liquid at an electron filling factor of 1/3 have been studied. It was found that the lowest in energy are spin-magnetogravitons, excitations with a simultaneous change in the electron density in the Laughlin liquid and the spin quantum number of the electron system. The experimental possibility of the formation of new quasi-equilibrium states of anionic matter – Laughlin solutions of spin-magnetogravitons – is demonstrated. A new type of optical scattering is observed in Laughlin solutions.

Novel dopant-free ferromagnetic Mott-like insulator and high-energy correlated-plasmons in unconventional strongly correlated s band of low-dimensional gold

Ferromagnetic insulators and plasmons have attracted a lot of interest due to their rich fundamental science and applications. Recent research efforts have been made to find dopant-free ferromagnetic insulators and unconventional plasmons independently both in strongly correlated electron systems. However, our understanding of them is still lacking. Existing dopant-free ferromagnetic insulator materials are mostly limited to complex d- or f-systems with extremely low Curie temperature, low-symmetry structure, and strict growth conditions on specific substrates, limiting their compatibility with industrial applications. Unconventional plasmon is, on the other hand, a quasiparticle that originates from the collective excitation of correlated-charges, yet they are rarely explored, particularly in ferromagnetic insulator materials. Herewith, we present a novel, room temperature dopant-free ferromagnetic Mott-like insulator with a high-symmetry structure in unconventional strongly correlated s band of low-dimensional highly oriented single-crystal gold quantum dots (HOSG-QDs) on MgO(001). Interestingly, HOSG-QDs show new high-energy correlated-plasmons with low-plasmonics-loss. With a series of state-of-the-art experimental techniques, we find that the Mott-insulating state is tunable with surprisingly strong spin-splitting and spin polarization accompanied by strong s–s transitions, disappearance of Drude response, and generating new Mott-like gap. Supported with a series of theoretical calculations, the interplay of quantum confinement, many-body electronic correlations, and hybridizations tunes electron–electron correlations in s band and determines the ferromagnetism, Mott-like insulator, and high-energy correlated-plasmons. Our result shows a new class of room temperature dopant-free ferromagnetic Mott-like insulator and high-energy correlated-plasmons with low-loss in strongly correlated s band and opens unexplored applications of low-dimensional gold in spin field-effect transistors and plasmonics.

Breaking Surface-Plasmon Excitation Constraint via Surface Spin Waves.

Surface plasmons in two-dimensional (2D) electron systems have attracted great attention for their promising light-matter applications. However, the excitation of a surface plasmon, in particular, transverse-electric (TE) surface plasmon, remains an outstanding challenge due to the difficulty to conserve energy and momentum simultaneously in the normal 2D materials. Here we show that the TE surface plasmons ranging from gigahertz to terahertz regime can be effectively excited and manipulated in a hybrid dielectric, 2D material, and magnet structure. The essential physics is that the surface spin wave supplements an additional freedom of surface plasmon excitation and thus greatly enhances the electric field in the 2D medium. Based on widely used magnetic materials like yttrium iron garnet and manganese difluoride, we further show that the plasmon excitation manifests itself as a measurable dip in the reflection spectrum of the hybrid system while the dip position and the dip depth can be well controlled by an electric gating on the 2D layer and an external magnetic field. Our findings should bridge the fields of low-dimensional physics, plasmonics, and spintronics and open a novel route to integrate plasmonic and spintronic devices.

New high-precision measurement system for electron–positron pairs from sub-GeV/GeV gamma-rays in the emulsion telescope

The GRAINE project observes cosmic gamma-rays, using a balloon-borne emulsion-film-based telescope in the sub-GeV/GeV energy band. We reported in our previous balloon experiment in 2018, GRAINE2018, the detection of the known brightest source, Vela pulsar, with the highest angular resolution ever reported in an energy range of >80MeV. However, the emulsion scanning system used in the experiment was designed to achieve a high-speed scanning, and it was not accurate enough to ensure the optimum spatial resolution of the emulsion film and limited the performance. Here, we report a new high-precision scanning system that can be used to greatly improve the observation result of GRAINE2018 and also be employed in future experiments. The scanning system involves a new algorithm that recognizes each silver grain on an emulsion film and is capable of measuring tracks with a positional resolution for the passing points of tracks of almost the same as the intrinsic resolution of nuclear emulsion film (∼70 nm). This resolution is approximately one order of magnitude smaller than that obtained with the high-speed scanning system. With this scanning system, an angular resolution for gamma-rays of 0.1° at 1GeV is expected to be achieved. Furthermore, we successfully combine the new high-precision scanning system with the existing high-speed scanning system, enabling the high-speed and high-precision measurements. Employing these techniques, we reanalyze the gamma-ray events detected previously by only the high-speed scanning system in GRAINE2018 and obtain an about three times higher angular resolution (0.22°) in the 500–700MeV energy range. Adopting this technique in future observations may provide new insights into the gamma-ray emission from the Galactic center region and may realize polarization measurements of high-energy cosmic gamma-rays.

Model and Energy Bounds for a Two-Dimensional System of Electrons Localized in Concentric Rings.

We study a two-dimensional system of interacting electrons confined in equidistant planar circular rings. The electrons are considered spinless and each of them is localized in one ring. While confined to such ring orbits, each electron interacts with the remaining ones by means of a standard Coulomb interaction potential. The classical version of this two-dimensional quantum model can be viewed as representing a system of electrons orbiting planar equidistant concentric rings where the kinetic energy may be discarded when one is searching for the lowest possible energy. Within this framework, the lowest possible energy of the system is the one that minimizes the total Coulomb interaction energy. This is the equilibrium energy that is numerically determined with high accuracy by using the simulated annealing method. This process allows us to obtain both the equilibrium energy and position configuration for different system sizes. The adopted semi-classical approach allows us to provide reliable approximations for the quantum ground state energy of the corresponding quantum system. The model considered in this work represents an interesting problem for studies of low-dimensional systems, with echoes that resonate with developments in nanoscience and nanomaterials.

Controlling orbital magnetism of band electron systems via bath engineering

Controlling orbital magnetism of band electron systems via bath engineering

Unveiling short-range magnetic correlations: The development of magnetic pair distribution function method at CSNS

Recent advancements in the magnetic pair distribution function (mPDF) analysis of neutron total scattering data provide a powerful approach to investigate local magnetic correlations in materials. This technique is promising for revealing short-range magnetic correlations at the sub-nanometer length scale directly in real space. It is particularly suitable for strongly correlated electron systems and geometrically frustrated magnets. In this study, the mPDF experiment is conducted at the multi-physics instrument (MPI) of the China Spallation Neutron Source, one of the latest neutron total scattering diffractometers in the world. We systematically benchmarked a series of important parameters related to the experimental setup and data processing for mPDF experiments at the MPI and similar instruments. This method not only advances the magnetic structure determination of fundamental materials but also opens the door for extending mPDF studies to more complicated and frontier magnetic systems that are challenging for conventional diffraction methods.

Study of the Singlet and the Triplet States of Two ElectronSystems in the First Excited State

A study of the singlet and triplet states of two electron systems in the first excited state was performed using a simple quantum mechanical model, which assigns the 1s,and 2s orbital with two different variational parameters. Our results agree with a high level calculation used by Snow and Bills.