Browse
Submit Data
Databases
API
Help

Dataset Information

0 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Electronic landscape of the f-electron intermetallics with the ThCr₂Si₂ structure.

ABSTRACT: 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 ThCr₂Si₂ 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.

SUBMITTER: Lai Y

PROVIDER: S-EPMC9365280 | biostudies-literature | 2022 Aug

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Publications

Electronic landscape of the f-electron intermetallics with the ThCr2Si2 structure.

Lai You Y Chan Julia Y JY Baumbach Ryan E RE

Science advances 20220810 32

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 ThCr2Si2 structu ...[more]

PMID: 35947661

Similar Datasets

Insight into the electronic structure of the centrosymmetric skyrmion magnet GdRu2Si2.

Project description:The discovery of a square magnetic-skyrmion lattice in GdRu2Si2, with the smallest so far found skyrmion size and without a geometrically frustrated lattice, has attracted significant attention. In this work, we present a comprehensive study of surface and bulk electronic structures of GdRu2Si2 by utilizing momentum-resolved photoemission (ARPES) measurements and first-principles calculations. We show how the electronic structure evolves during the antiferromagnetic transition when a peculiar helical order of 4f magnetic moments within the Gd layers sets in. A nice agreement of the ARPES-derived electronic structure with the calculated one has allowed us to characterize the features of the Fermi surface (FS), unveil the nested region along kz at the corner of the 3D FS, and reveal their orbital compositions. Our findings suggest that the Ruderman-Kittel-Kasuya-Yosida interaction plays a decisive role in stabilizing the spiral-like order of Gd 4f moments responsible for the skyrmion physics in GdRu2Si2. Our results provide a deeper understanding of electronic and magnetic properties of this material, which is crucial for predicting and developing novel skyrmion-based systems.

| S-EPMC10662135 | biostudies-literature

Electronic Structure of In3-x Se4 Electron Transport Layer for Chalcogenide/p-Si Heterojunction Solar Cells.

Project description:In this article, we perform density functional theory calculation to investigate the electronic and optical properties of newly reported In3-x Se4 compound using CAmbridge Serial Total Energy Package (CASTEP). Structural parameters obtained from the calculations agree well with the available experimental data, indicating their stability. In the band structure of In3-x Se4 (x = 0, 0.11, and, 0.22), the Fermi level (E F) crossed over several bands in the conduction bands, which is an indication of the n-type metal-like behavior of In3-x Se4 compounds. On the other hand, the band structure of In3-x Se4 (x = 1/3) exhibits semiconducting nature with a band gap of ∼0.2 eV. A strong hybridization among Se 4s, Se 4p and In 5s, In 5p orbitals for In3Se4 and that between Se 4p and In 5p orbitals were seen for β-In2Se3 compound. The dispersion of In 5s, In 5p and Se 4s, Se 4p orbitals is responsible for the electrical conductivity of In3Se4 that is confirmed from DOS calculations as well. Moreover, the bonding natures of In3-x Se4 materials have been discussed based on the electronic charge density map. Electron-like Fermi surface in In3Se4 ensures the single-band nature of the compound. The efficiency of the In3-x Se4/p-Si heterojunction solar cells has been calculated by Solar Cell Capacitance Simulator (SCAPS)-1D software using experimental data of In3-x Se4 thin films. The effect of various physical parameters on the photovoltaic performance of In3-x Se4/p-Si solar cells has been investigated to obtain the highest efficiency of the solar cells. The optimized power conversion efficiency of the solar cell is found to be 22.63% with V OC = 0.703 V, J SC = 38.53 mA/cm2, and FF = 83.48%. These entire theoretical predictions indicate the promising applications of In3-x Se4 two-dimensional compound to harness solar energy in near future.

| S-EPMC6822117 | biostudies-literature

Electronic strengthening mechanism of covalent Si via excess electron/hole doping.

Project description:Brittle fracture of a covalent material is ultimately governed by the strength of the electronic bonds. Recently, attempts have been made to alter the mechanical properties including fracture strength by excess electron/hole doping. However, the underlying mechanics/mechanism of how these doped electrons/holes interact with the bond and changes its strength is yet to be revealed. Here, we perform first-principles density-functional theory calculations to clarify the effect of excess electrons/holes on the bonding strength of covalent Si. We demonstrate that the bond strength of Si decreases or increases monotonically in correspondence with the doping concentration. Surprisingly, change to the extent of 30-40% at the maximum feasible doping concentration could be observed. Furthermore, we demonstrated that the change in the covalent bond strength is determined by the bonding/antibonding state of the doped excess electrons/holes. In summary, this work explains the electronic strengthening mechanism of covalent Si from a quantum mechanical point of view and provides valuable insights into the electronic-level design of strength in covalent materials.

| S-EPMC10545711 | biostudies-literature

Si Doping-Induced Electronic Structure Regulation of Single-Atom Fe Sites for Boosted CO2 Electroreduction at Low Overpotentials.

Project description:Transition metal-based single-atom catalysts (TM-SACs) are promising alternatives to Au- and Ag-based electrocatalysts for CO production through CO2 reduction reaction. However, developing TM-SACs with high activity and selectivity at low overpotentials is challenging. Herein, a novel Fe-based SAC with Si doping (Fe-N-C-Si) was prepared, which shows a record-high electrocatalytic performance toward the CO2-to-CO conversion with exceptional current density (>350.0 mA cm-2) and ~100% Faradaic efficiency (FE) at the overpotential of <400 mV, far superior to the reported Fe-based SACs. Further assembling Fe-N-C-Si as the cathode in a rechargeable Zn-CO2 battery delivers an outstanding performance with a maximal power density of 2.44 mW cm-2 at an output voltage of 0.30 V, as well as high cycling stability and FE (>90%) for CO production. Experimental combined with theoretical analysis unraveled that the nearby Si dopants in the form of Si-C/N bonds modulate the electronic structure of the atomic Fe sites in Fe-N-C-Si to markedly accelerate the key pathway involving *CO intermediate desorption, inhibiting the poisoning of the Fe sites under high CO coverage and thus boosting the CO2RR performance. This work provides an efficient strategy to tune the adsorption/desorption behaviors of intermediates on single-atom sites to improve their electrocatalytic performance.

| S-EPMC10017332 | biostudies-literature

All-Electron Plane-Wave Electronic Structure Calculations.

Project description:We demonstrate the use of the plane wave basis for all-electron electronic structure calculations. The approach relies on the definition of an analytic, norm-conserving, regularized Coulomb potential, and a scalable implementation of the plane wave method capable of handling large energy cutoffs (up to 80 kRy in the examples shown). The method is applied to the computation of electronic properties of isolated atoms as well as the diamond and silicon crystals, MgO, solid argon, and a configuration of 64 water molecules extracted from a first-principles molecular dynamics simulation. The computed energies, band gaps, ionic forces, and stress tensors provide reference results for the validation of pseudopotentials and/or localized basis sets. A calculation of the all-electron band structure of diamond and silicon using the SCAN meta-GGA density functional allows for a validation of calculations based on pseudopotentials derived using the PBE exchange-correlation functional. In the case of (H2O)64, the computed ionic forces provide a reference from which the errors incurred in pseudopotential calculations and in localized Gaussian basis sets calculations can be estimated.

| S-EPMC9979607 | biostudies-literature

Superconductivity-Electron Count Relationship in Heusler Phases-the Case of LiPd2Si.

Project description:We report superconductivity in the full Heusler compound LiPd2Si (space group Fm3̅m, No. 225) at a critical temperature of Tc = 1.3 K and a normalized heat capacity jump at Tc, ΔC/γTc = 1.1. The low-temperature isothermal magnetization curves imply type-I superconductivity, as previously observed in LiPd2Ge. We show, based on density functional theory calculations and using the molecular orbital theory approach, that while LiPd2Si and LiPd2Ge share the Pd cubic cage motif that is found in most of the reported Heusler superconductors, they show distinctive features in the electronic structure. This is due to the fact that Li occupies the site which, in other compounds, is filled with an early transition metal or a rare-earth metal. Thus, while a simple valence electron count-property relationship is useful in predicting and tuning Heusler materials, inclusion of the symmetry of interacting frontier orbitals is also necessary for the best understanding.

| S-EPMC10902818 | biostudies-literature

Superconducting YAu3Si and Antiferromagnetic GdAu3Si with an Interpenetrating Framework Structure Built from 16-Atom Polyhedra.

Project description:Investigations of reaction mixtures REx(Au0.79Si0.21)100-x (RE = Y and Gd) yielded the compounds REAu3Si which adopt a new structure type, referred to as GdAu3Si structure (tP80, P42/mnm, Z = 16, a = 12.8244(6)/12.7702(2) Å, and c = 9.0883(8)/9.0456(2) Å for GdAu3Si/YAu3Si, respectively). REAu3Si was afforded as millimeter-sized faceted crystal specimens from solution growth employing melts with composition RE18(Au0.79Si0.21)82. In the GdAu3Si structure, the Au and Si atoms are strictly ordered and form a framework built of corner-connected, Si-centered, trigonal prismatic units SiAu6. RE atoms distribute on 3 crystallographically different sites and each attain a 16-atom coordination by 12 Au and 4 Si atoms. These 16-atom polyhedra commonly fill the space of the unit cell. The physical properties of REAu3Si were investigated by heat capacity, electrical resistivity, and magnetometry techniques and are discussed in the light of theoretical predictions. YAu3Si exhibits superconductivity around 1 K, whereas GdAu3Si shows a complex magnetic ordering, likely related to frustrated antiferromagnets exhibiting chiral spin textures. GdAu3Si-type phases with interesting magnetic and transport properties may exist in an extended range of ternary RE-Au-Si systems, similar to the compositionally adjacent cubic 1/1 approximants RE(Au,Si)∼6.

| S-EPMC8924926 | biostudies-literature

Crystal Structure and Ferromagnetism of the CeFe9Si4 Intermetallic Compound.

Project description:We have determined the crystal structure and the magnetic state of the CeFe9Si4 intermetallic compound. Our revised structural model (fully ordered tetragonal unit cell, I4/mcm) agrees with the previous literature report, except for some minor quantitative differences. Magnetically, the CeFe9Si4 undergoes a ferromagnetic transition at the temperature TC ≈ 94 K. Ferromagnetism in the combined Ce-Fe spin system is a result of interplay between the localized magnetism of the Ce sublattice and the Fe band (itinerant) magnetism. Ferromagnetic ordering obeys the rather general rule that the exchange spin coupling between atoms possessing more than half-full d shells with atoms possessing less than half-full d shells is antiferromagnetic (where the Ce atoms are considered as light d elements). Since in rare-earth metals from the light half of the lanthanide series, the magnetic moment is directed opposite to the spin, this results in ferromagnetism. The magnetoresistance and the magnetic specific heat show an additional temperature-dependent feature (a shoulder) deep inside the ferromagnetic phase that is considered to originate from the influence of the magnetization on the electronic band structure via the magnetoelastic coupling, which alters the Fe band magnetism below TC. The ferromagnetic phase of CeFe9Si4 is magnetically soft.

| S-EPMC10114074 | biostudies-literature

Electrically-triggered micro-explosion in a graphene/SiO2/Si structure.

Project description:Electrically-triggered micro-explosions in a metal-insulator-semiconductor (MIS) structure can fragment/atomize analytes placed on it, offering an interesting application potential for chip-scale implementation of atomic emission spectroscopy (AES). We have investigated the mechanisms of micro-explosions occurring in a graphene/SiO2/Si (GOS) structure under a high-field pulsed voltage drive. Micro-explosions are found to occur more readily in inversion bias than in accumulation bias. Explosion damages in inversion-biased GOS differ significantly between n-Si and p-Si substrate cases: a highly localized, circular, protruding cone-shape melt of Si for the n-Si GOS case, whereas shallow, irregular, laterally-propagating trenches in SiO2/Si for the p-Si GOS case. These differing damage morphologies are explained by different carrier-multiplication processes: in the n-Si case, impact ionization propagates from SiO2 to Si, causing highly-localized melt explosions of Si in the depletion region, whereas in the p-Si case, from SiO2 towards graphene electrode, resulting in laterally wide-spread micro-explosions. These findings are expected to help optimize the GOS-based atomizer structure for low voltage, small-volume analyte, high sensitivity chip-scale emission spectroscopy.

| S-EPMC5943326 | biostudies-literature

High Electron Mobility in Si-Doped Two-Dimensional β-Ga2O3 Tuned Using Biaxial Strain.

Project description:Two-dimensional (2D) semiconductors have attracted much attention regarding their use in flexible electronic and optoelectronic devices, but the inherent poor electron mobility in conventional 2D materials severely restricts their applications. Using first-principles calculations in conjunction with Boltzmann transport theory, we systematically investigated the Si-doped 2D β-Ga2O3 structure mediated by biaxial strain, where the structural stabilities were determined by formation energy, phonon spectrum, and ab initio molecular dynamic simulation. Initially, the band gap values of Si-doped 2D β-Ga2O3 increased slightly, followed by a rapid decrease from 2.46 eV to 1.38 eV accompanied by strain modulations from -8% compressive to +8% tensile, which can be ascribed to the bigger energy elevation of the σ* anti-bonding in the conduction band minimum than that of the π bonding in the valence band maximum. Additionally, band structure calculations resolved a direct-to-indirect transition under the tensile strains. Furthermore, a significantly high electron mobility up to 4911.18 cm2 V-1 s-1 was discovered in Si-doped 2D β-Ga2O3 as the biaxial tensile strain approached 8%, which originated mainly from the decreased quantum confinement effect on the surface. The electrical conductivity was elevated with the increase in tensile strain and the enhancement of temperature from 300 K to 800 K. Our studies demonstrate the tunable electron mobilities and band structures of Si-doped 2D β-Ga2O3 using biaxial strain and shed light on its great potential in nanoscale electronics.

| S-EPMC11356731 | biostudies-literature