Hubbard parameters for programmable tweezer arrays
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Wei, Hao-Tian (ORCID:0000000176842608)↗
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Results for “Hubbard parameter”
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Machine learning the Hubbard U parameter in DFT+U using Bayesian optimization
Abstract Within density functional theory (DFT), adding a Hubbard U correction can mitigate some of the deficiencies of local and semi-local exchange-correlation functionals, while maintaining computational efficiency. However, the accuracy of DFT+U largely depends on the chosen Hubbard U values. We propose an approach to determining the optimal U parameters for a given material by machine learning. The Bayesian optimization (BO) algorithm is used with an objective function formulated to reproduce the band structures produced by more accurate hybrid functionals. This approach is demonstrated for transition metal oxides, europium chalcogenides, and narrow-gap semiconductors. The band structures obtained using the BO U values are in agreement with hybrid functional results. Additionally, comparison to the linear response (LR) approach to determining U demonstrates that the BO method is superior.
Chemistry↗
Theoretical predictive screening of noble-metal-containing M 3 AuC 2 (M = Ti, V, and Cr) MAX phases
Using first-principles density functional theory (DFT), the ground state physical properties of the newly synthesized noble-metal-containing Ti 3 AuC 2 MAX phase have been investigated. The effect of transition-element Ti replacement (V and Cr) on physical properties, including structural, elastic, electronic, thermal, and optical are presented. The optimized lattice parameters of Ti 3 AuC 2 MAX phase are in good agreement with the experimental values and decrease when we replace Ti with V and then Cr. The magnetic properties of M 3 AuC 2 are predicted by using generalized gradient approximation (GGA) incorporating onsite electron correlation parameter (Hubbard U parameter) within DFT. Out of three studied MAX phases, V 3 AuC 2 and Cr 3 AuC 2 phases exhibit magnetism. The thermodynamical stability of M 3 AuC 2 (M = Ti, V, and Cr) phases is discussed by the formation enthalpy with respect to their most competing phases. The electronic structure reveals that these phases have metallic nature and are electrically anisotropic. The M-element replacement has an effect on the bonding properties of M 3 AuC 2 . The bonding between M-C is in the order of Cr 3 AuC 2 > V 3 AuC 2 > Ti 3 AuC 2 according to their peak positions and heights of density of states in the occupied site, which is also confirmed from the charge density distribution. The elastic properties indicate that M 3 AuC 2 phases are ductile, machinable, less stiff, and better resistant to thermal shock and are elastically anisotropic. To understand the properties of M 3 AuC 2 for the extreme environment, we employed a quasi-harmonic Debye model at the pressure and temperature range of 0–50 GPa and 0–1600 K, respectively. Additionally, we evaluated thermal conductivity and melting temperature to further understand the potential of these MAX phases in coating applications at elevated temperature. In relation to optical properties, these MAX phases have a reasonable absorption coefficient in the visible as well as in the ultra-violet regions. The reflectivity of M 3 AuC 2 phases is polarization dependent and of 45 % against the visible region, which reveals its potential as coating material to minimize solar heating.
312 MAX phases↗
Improving gas adsorption modeling for MOFs by local calibration of Hubbard U parameters
While computational screening with density functional theory (DFT) is frequently employed for the screening of metal–organic frameworks (MOFs) for gas separation and storage, commonly applied generalized gradient approximations (GGAs) exhibit self-interaction errors, which hinder the predictions of adsorption energies. We investigate the Hubbard U parameter to augment DFT calculations for full periodic MOFs, targeting a more precise modeling of gas molecule–MOF interactions, specifically for N2, CO2, and O2. We introduce a calibration scheme for the U parameter, which is tailored for each MOF, by leveraging higher-level calculations on the secondary building unit (SBU) of the MOF. When applied to the full periodic MOF, the U parameter calibrated against hybrid HSE06 calculations of SBUs successfully reproduces hybrid-quality calculations of the adsorption energy of the periodic MOF. The mean absolute deviation of adsorption energies reduces from 0.13 eV for a standard GGA treatment to 0.06 eV with the calibrated U, demonstrating the utility of the calibration procedure when applied to the full MOF structure. Furthermore, attempting to use coupled cluster singles and doubles with perturbative triples calculations of isolated SBUs for this calibration procedure shows varying degrees of success in predicting the experimental heat of adsorption. It improves accuracy for N2 adsorption for cases of overbinding, whereas its impact on CO2 is minimal, and ambiguities in spin state assignment hinder consistent improvements of O2 adsorption. Our findings emphasize the limitations of cluster models and advocate the use of full periodic MOF systems with a calibrated U parameter, providing a more comprehensive understanding of gas adsorption in MOFs.
Chemistry↗
LDA + $U_{sc}$ calculations of phase relations in FeO
Using the LDA + $U_{sc}$ method, we present calculation phase relations of iron monoxides involving five polytypes in multiple spin-state configurations. In this work, the Hubbard parameter $\textit{U}$ is determined self-consistently simultaneously with the occupation matrix and structures at arbitrary pressures. The Hubbard parameter strongly depends on pressure, structure, and spin state. Comparison with experimental structural data indicates the LDA + $U_{sc}$ can predict structure, compression curves, phase relations, and transition pressures very well for the insulating $\textit{B}$1 and $\textit{iB}$8 states. However, it requires additional calculations using the Mermin functional that includes the electronic entropic contribution to the free energy to obtain an $\textit{nB}$8 metallic state and a consistent $\textit{iB}$8 to $\textit{nB}$8 insulator to metal transition pressure.
36 MATERIALS SCIENCE↗
Rationalization of the Hubbard U parameter in CeO{sub x} from first principles: Unveiling the role of local structure in screening
The density functional theory (DFT)+U method has been widely employed in theoretical studies on various ceria systems to correct the delocalization bias in local and semi-local DFT functionals with moderate computational cost. We present a systematic and quantitative study, aiming to gain better understanding of the dependence of Hubbard U on the local atomic arrangement. To rationalize the Hubbard U of Ce 4f, we employed the first principles linear response method to compute Hubbard U for Ce in ceria clusters, bulks, and surfaces. We found that the Hubbard U varies in a wide range from 4.3 eV to 6.7 eV, and exhibits a strong correlation with the Ce coordination number and Ce–O bond lengths, rather than the Ce 4f valence state. The variation of the Hubbard U can be explained by the changes in the strength of local screening due to O → Ce intersite transitions.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Combined hybrid functional and DFT+U calculations for metal chalcogenides
In the density-functional studies of materials with localized electronic states, the local/semilocal exchange-correlation functionals are often either combined with a Hubbard parameter U as in the LDA+U method or mixed with a fraction of exactly computed (Fock) exchange energy yielding a hybrid functional. Although some inaccuracies of the semilocal density approximations are thus fixed to a certain extent, the improvements are not sufficient to make the predictions agree with the experimental data. Here, we put forward the perspective that the hybrid functional scheme and the LDA+U method should be treated as complementary, and propose to combine the range-separated Heyd-Scuseria-Ernzerhof (HSE) hybrid functional with the Hubbard U. We thus present a variety of HSE+U calculations for a set of II-VI semiconductors, consisting of zinc and cadmium monochalcogenides, along with comparison to the experimental data. Our findings imply that an optimal value U{sup *} of the Hubbard parameter could be determined, which ensures that the HSE+U{sup *} calculation reproduces the experimental band gap. It is shown that an improved description not only of the electronic structure but also of the crystal structure and energetics is obtained by adding the U{sup *} term to the HSE functional, proving the utility of HSE+U{sup *} approach in modeling semiconductors with localized electronic states.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Electronic and magnetic properties of double perovskite Dy{sub 2}MnCoO{sub 6} by first-principles calculation
Using first-principles calculation, we investigate electronic and magnetic properties of Dy{sub 2}MnCoO{sub 6}. A detailed structural optimization has been done and found that the orthorhombic structure with Mn (Co) ions aligning along the longest axis type is the most stable structure. Within the generalized gradient approximation, the spin polarized calculations predict Dy{sub 2}MnCoO{sub 6} to be a half-metallic with ferromagnetic interaction between Mn and Co ions and antiferromagnetic interaction between Dy and Mn/Co ions. We also investigate the effect of Hubbard parameter (U) on the ground state magnetic structure. For all values of Hubbard U parameter the Co ions have nonzero magnetic moment; they do not lie in low-spin state, as in DyCoO{sub 3}.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Signatures of tunable superconductivity in a trilayer graphene moiré superlattice
Understanding the mechanism of high-transition-temperature (high-T c ) superconductivity is a central problem in condensed matter physics. It is often speculated that high-Tc superconductivity arises in a doped Mott insulator1 as described by the Hubbard model 2,3,4 . An exact solution of the Hubbard model, however, is extremely challenging owing to the strong electron–electron correlation in Mott insulators. Therefore, it is highly desirable to study a tunable Hubbard system, in which systematic investigations of the unconventional superconductivity and its evolution with the Hubbard parameters can deepen our understanding of the Hubbard model. Here we report signatures of tunable superconductivity in an ABC-trilayer graphene (TLG) and hexagonal boron nitride (hBN) moiré superlattice. Unlike in ‘magic angle’ twisted bilayer graphene, theoretical calculations show that under a vertical displacement field, the ABC-TLG/hBN heterostructure features an isolated flat valence miniband associated with a Hubbard model on a triangular superlattice 5,6 where the bandwidth can be tuned continuously with the vertical displacement field. Upon applying such a displacement field we find experimentally that the ABC-TLG/hBN superlattice displays Mott insulating states below 20 kelvin at one-quarter and one-half fillings of the states, corresponding to one and two holes per unit cell, respectively. Upon further cooling, signatures of superconductivity (‘domes’) emerge below 1 kelvin for the electron- and hole-doped sides of the one-quarter-filling Mott state. The electronic behaviour in the ABC-TLG/hBN superlattice is expected to depend sensitively on the interplay between the electron–electron interaction and the miniband bandwidth. By varying the vertical displacement field, we demonstrate transitions from the candidate superconductor to Mott insulator and metallic phases. Our study shows that ABC-TLG/hBN heterostructures offer attractive model systems in which to explore rich correlated behaviour emerging in the tunable triangular Hubbard model.
36 MATERIALS SCIENCE↗
The Effects of Ru and Rh Substitutions on the Magneto-electronic and Optical Properties of the TbNi{sub 5} Intermetallic Compound: An Ab Initio Investigation
In this study, we have performed the first-principles investigation of the structural, electronic, magnetic, and optical properties of TbNi{sub 5}, TbNi{sub 3}Ru{sub 2}, and TbNi{sub 3}Rh{sub 2} compounds. The full-potential linearized augmented plane waves with local orbitals method is used in the framework of density functional theory (DFT) employing the generalized gradient approximation (GGA) for the exchange correlation functional as implemented in WIEN2k package. The structural properties are reposed on the evaluation of the equilibrium lattice parameters of these compounds under hexagonal structure such as lattice constants (a and c), bulk modulus (B), and its first pressure derivative (B{sup ′}). The spin-polarized electronic structures, including band structure and density of states, are calculated employing the GGA plus band correlated Hubbard parameter (GGA + U) scheme. The results show that density of states and magnetic moment of the pure TbNi{sub 5} compound are changed by doping. These changes are observed in the appearance of additional peaks on the spectral density of states (DOS) and in the augmentation of the total magnetic moment of TbNi{sub 3}X{sub 2} (X = Ru and Rh) intermetallic compounds. Based on the electronic structure results, the frequency dependents of optical conductivity are estimated in all the spectra and interpreted in the interband optical absorption part.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Crystal and Electronic Structures of Neptunium Nitrides Synthesized Using a Fluoride Route
A low-temperature fluoride route was utilized to synthesize neptunium mononitride, NpN. Through the development of this process, two new neptunium nitride species, NpN{sub 2} and Np{sub 2}N{sub 3}, were identified. The NpN{sub 2} and Np{sub 2}N{sub 3} have crystal structures isomorphous to those of UN{sub 2} and U{sub 2}N{sub 3}, respectively. NpN{sub 2} crystallizes in a face-centered cubic CaF{sub 2}-type structure with a space group of Fm3m and a refined lattice parameter of 5.3236(1) {angstrom}. The Np{sub 2}N{sub 3} adopts the body-centered cubic Mn{sub 2}O{sub 3}-type structure with a space group of Ia{bar 3}. Its refined lattice parameter is 10.6513(4) {angstrom}. The NpN synthesis at temperatures {le} 900 C using the fluoride route discussed here was also demonstrated. Previous computational studies of the neptunium nitride system have focused exclusively on the NpN phase because no evidence was reported experimentally on the presence of NpN{sub x} systems. Here, the crystal structures of NpN{sub 2} and Np{sub 2}N{sub 3} are discussed for the first time, confirming the experimental results by density functional calculations (DFT). These DFT calculations were performed within the local-density approximation (LDA+U) and the generalized-gradient approximation (GGA+U) corrected with an effective Hubbard parameter to account for the strong on-site Coulomb repulsion between Np 5f electrons. The effects of the spin-orbit coupling in the GGA+U calculations have also been investigated for NpN{sub 2} and NpN.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Specific features of insulator-metal transitions under high pressure in crystals with spin crossovers of 3d ions in tetrahedral environment
For Mott insulators with tetrahedral environment, the effective Hubbard parameter U{sub eff} is obtained as a function of pressure. This function is not universal. For crystals with d{sup 5} configuration, the spin crossover suppresses electron correlations, while for d{sup 4} configurations, the parameter U{sub eff} increases after a spin crossover. For d{sup 2} and d{sup 7} configurations, U{sub eff} increases with pressure in the high-spin (HS) state and is saturated after the spin crossover. Characteristic features of the insulator-metal transition are considered as pressure increases; it is shown that there may exist cascades of several transitions for various configurations.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Analysis of the sequence of insulator-metal phase transitions at high pressure in systems with spin crossovers
Possible variants of the Mott-Hubbard phase transitions at high pressure in systems with spin crossovers are considered. Owing to the universal character of the dependence of the effective Hubbard parameter U{sub eff}(d{sup n}) on the average number of d electrons, which is determined by the presence of spin crossovers, cascades of insulator-metal-insulator phase transitions in systems with d{sup 3}, d{sup 6}, and d{sup 8} configurations become possible. Moreover, the systems with d{sup 6} configuration can exhibit transitions from a metal in the absence of external pressure to an insulator at high pressure.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Unraveling Site Selective Magnetic Properties of Cobalt Sites in Critical Elements Lean RE(TM)5 Magnet Materials
We report here our discovery of crystallographic and interstitial sites and onsite electron correlation propelled intrinsic and derived permanent magnetic properties of critical elements lean RE(TM) 5 (RE = La, Ce and TM = Fe, Co) magnet materials. A full potential linearized augmented plane wave (FP-LAPW) method within the local density approximation (LDA) is used to investigate and analyze the electronic structure and magnetism of these RE(TM) 5 type structures. To better correlate the experimental results, the effective Coulomb (U) and exchange (J) interactions (Hubbard parameters) are crucial at the transition metal sites. Results show that the main propeller of magnetic anisotropy in these compounds is the cobalt atoms at the 2c sites not the 3g sites. This site-specific property and site preference energetics are used to replace 3g sites with non-critical elements such as iron that exhibits a larger magnetic moment. Based on this strategic replacement, we predict two new compounds that have a larger hardness parameter with a relatively large energy product due to the atomic dilution caused by interstitial addition of nitrogen in the compounds: CeCo 2 Fe 3 N 2 and LaCo 2 Fe 3 N 2 .
Rare-earths↗
Magneto-induced tunability of thermo-spin current in deformed zigzag graphene nanoribbons
The aim of this report is to unfold how the thermo-electric spin-polarized current in a transverse-biased zigzag graphene nanoribbon changes in the presence of uniaxial deformations and uniform perpendicular magnetic field. Employing the two-parameter Hubbard model along with the non-equilibrium Green's function formalism, we found that both uniaxial strain and magnetic field can significantly modulate the bandgap, local distribution of edge states, and the critical transverse electric field needed to achieve the half-metallic phase in the ribbon. Our analysis shows a significant enhancement of the maximum attainable spin-polarized current as functions of both source temperature and contacts temperature difference, with increasing the magnetic field or applying any magnitude of compressive strain. Furthermore, it is shown that the magneto-resistance ratio of the device, can be drastically tuned via strain engineering, reaching values as high as 2 × 10{sup 4}% for compressive strains of 5% magnitude.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Ab initio study of vacancy formation in cubic LaMnO{sub 3} and SmCoO{sub 3} as cathode materials in solid oxide fuel cells
Doped LaMnO{sub 3} and SmCoO{sub 3} are important solid oxide fuel cell cathode materials. The main difference between these two perovskites is that SmCoO{sub 3} has proven to be a more efficient cathode material than LaMnO{sub 3} at lower temperatures. In order to explain the difference in efficiency, we need to gain insight into the materials’ properties at the atomic level. However, while LaMnO{sub 3} has been widely studied, ab initio studies on SmCoO{sub 3} are rare. Hence, in this paper, we perform a comparative DFT + U study of the structural, electronic, and magnetic properties of these two perovskites. To that end, we first determined a suitable Hubbard parameter for the Co d–electrons to obtain a proper description of SmCoO{sub 3} that fully agrees with the available experimental data. We next evaluated the impact of oxygen and cation vacancies on the geometry, electronic, and magnetic properties. Oxygen vacancies strongly alter the electronic and magnetic structures of SmCoO{sub 3}, but barely affect LaMnO{sub 3}. However, due to their high formation energy, their concentrations in the material are very low and need to be induced by doping. Studying the cation vacancy concentration showed that the formation of cation vacancies is less energetically favorable than oxygen vacancies and would thus not markedly influence the performance of the cathode.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Interplay between electron localization, magnetic order, and Jahn-Teller distortion dictates LiMnO2 phase stability
The development of manganese (Mn)-rich cathodes for Li-ion batteries promises to alleviate potential supply chain bottlenecks in battery manufacturing. Fundamental challenges in Mn-rich cathodes arise from phenomena such as structural changes due to cooperative Jahn-Teller (JT) distortions of in octahedral environments, Mn migration, and phase transformations to spinel-like order, all of which affect the electrochemical performance. These physically complex phenomena motivate an re-examination of the Li-Mn-O rock-salt space, with a focus on the thermodynamics of the prototypical, polymorphs. It is found that the generalized gradient approximation (GGA-PBEsol) and meta-GGA ( ) density functionals with empirically fitted on-site Hubbard corrections yield spurious stable phases for , such as predicting a phase with -like order ( ) to be the ground state instead of the orthorhombic (Pmmn) phase, which is the experimentally known ground state. Accounting for antiferromagnetic order in each structure is shown to have a substantial effect on the total energies and resulting phase stability. By using hybrid-GGA (HSE06) and GGA with self-consistent Hubbard parameters (on-site and inter-site ) calculated from linear response theory, the experimentally observed phase stability trends are recovered. The calculated on-site between Mn- states in the experimentally observed orthorhombic, layered, and spinel phases are significantly smaller than in and disordered layered structures, by within GGA. The smaller values of are shown to be correlated with a collinear ordering of JT distortions, in which all orbitals are oriented in the same direction. This cooperative JT effect can lead to greater electron delocalization from Mn along the states due to increased Mn-O covalency, which contributes to the greater electronic stability compared to the phases with noncollinear JT arrangements. The structures with collinear ordering of JT distortions also generate greater vibrational entropy, which helps stabilize these phases at high temperature. These phases are shown to be strongly insulating with large calculated band gaps , which are computed using HSE06 and .
Kam, Ronald L↗
Anisotropy and orbital moment in Sm-Co permanent magnets
Structural and magnetic properties of iron-free and iron-substituted SmCo 5 have been investigated theoretically and experimentally. The nanocrystalline ribbons of SmCo 5–x Fe x (0 ≤ x ≤ 2), which were produced by rapid solidification, crystallize in the hexagonal CaCu5 structure for x ≤ 0.75. Small Fe additions (x = 0.25) substantially improve the coercivity, from 0.45 to 2.70 T, which we interpret as combined intrinsic and extrinsic effect. Most of our findings are consistent with past samarium-cobalt research, but some are at odds with findings that have seemingly been well established through decades of rare-earth transition-metal research. In particular, our local spin-density approximation with Hubbard parameter calculations indicate that the electronic structure of the Sm atoms violates Hund's rules and that the orbital moment is strongly quenched. Possible reasons for the apparent disagreement between theory and experiment are discussed. Here, we explicitly determine the dependence of the Sm 4$f$ charge distribution, arguing that an accurate density-functional description of SmCo 5 is a challenge to future research.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗