Self-consistent Calculations Research Articles

Exploring Co2TiRE (RE = Nd and Tb) as a promising shape memory alloy using DFT methods

Our study employs self-consistent ab-initio calculations using highly precise spin-polarized density functional theory with both GGA and GGA+U approaches, coupled with the Boltzmann transport scheme. This comprehensive approach investigated the structural stability, magneto-electronic behavior, thermophysical characteristics, and thermoelectric transport properties of Co2TiRE (RE = Nd, Tb) Heusler alloys. Through structural optimizations, we confirm that these materials exhibit ferromagnetic behavior. Analysis of band occupation and density of states using GGA and GGA+U methods reveals that both compounds are metallic in both spin configurations. We evaluated key transport properties such as the Seebeck coefficient, electrical and thermal conductivity and the figure of merit to understand their potential in thermoelectric applications. Conservative estimates of the Seebeck coefficient and the figure of merit suggest promising applications in thermoelectric energy harvesting technologies. Additionally, we provide a comprehensive analysis of the thermophysical behavior, including the Debye temperature, thermal expansion, and specific heat, to assess the alloys thermodynamic stability across varying temperature and pressure conditions.

Analysis of the high-temperature transport property in GaN-based single and double heterostructures

GaN-based heterostructures have been proved to be excellent candidates for high-voltage, large-power, high-frequency and high-temperature application fields, thanks to their superior material properties. To further improve the carriers’ confinement, using InGaN channel layer or introducing AlGaN back barrier layer is promoted. These structures are also proved to be favorable for the robust electron mobility at high temperature. However, the reason solely rests on the longitudinal optical (LO) phonon scattering and the behind mechanism is still absent. This work compares the temperature-dependent electronic transport properties in three groups of GaN-based heterostructures, including GaN-based single heterostructure (SH) with/without AlN interlayer, GaN-based SH and double heterostructure (DH), and GaN-based DH with AlGaN or GaN channel layer. The advantageous high-temperature mobility is attributed to the enhanced LO phonon energy in heterostructures. By self-consistent calculations of the Schrödinger–Poisson equations, a close relation between the narrow electron distribution in the quantum well with the high LO phonon energy, and consequently superior mobility at high temperature is implied. The results provide a simple strategy for the optimized design of the GaN-based heterostructures outperforming at high temperature.

Evaluation of elastic constants of M23C6 and M7C3 embedded in Fe-Cr-C alloys using in-situ XRD tensile test and self-consistent model

This paper investigates the elastic properties of the model Fe-Cr-C alloys, specifically focusing on M23C6 and M7C3. The study uses in-situ synchrotron X-ray data during tensile deformation to determine the individual elastic characteristics of the matrix and iron/chromium carbides. The experimental results obtained from in-situ X-ray diffraction (XRD) are compared to the elastic constants of carbides that were reported in previous studies and derived using density function theory (DFT). The appropriate elastic constants for M23C6 and M7C3 were selected based on the self-consistent code executing with reported elastic constants. The directional elastic modulus and Poisson's ratio of iron/chromium carbides are calculated, and the anisotropy of the elastic constants is evaluated using the XRD lattice deformations under loading. The elastic modulus of carbide varies with the volume fraction of carbide in the effective medium. The study finds that the hexagonal structure is more probable than orthorhombic structure for M7C3 due to well-matched estimations of the directional elastic modulus and Poisson's ratio obtained from in-situ XRD data and the self-consistent calculations. In-situ XRD analysis of elastic behavior of each diffraction can be used to demonstrate the elastic constants of carbides and shows potential for obtaining precise elastic constants by integrating with self-consistent modeling and DFT.

Using ground state and excited state density functional theory to decipher 3d dopant defects in GaN

Using ground state density functional theory (DFT) and implementing an occupation-constrained DFT (occ-DFT) for self-consistent excited state calculations, we decipher the electronic structure of the Mn dopant and other 3ddefects in GaN across the band gap. Our analysis, validated with broad agreement with defect levels (ground-state calculations) and photoluminescence data (excited-state calculations), mandates reinterpretation and reassignment of 3ddefect data in GaN. The MnGadefect is determined to span stable charge states from (1-) inn-type GaN through (2+) inp-type GaN. The Mn(2+) is predicted to be ad2ground state spin triplet defect with a singlet excited state, isoelectronic with the defect associated with the 1.19 eV photoluminescence inn-type GaN. The combined analysis of defect levels and excited states invites reassessment of alld2-capable dopants in GaN. We demonstrate that the 1.19 eV defect, a candidate defect for optically controlled quantum applications, cannot be the Cr(1+) assumed in literature and instead must be the V(0). The combined ground-state/excited-state DFT analysis is shown to be able to chemically fingerprint defects.

Charge self-consistent dynamical mean field theory calculations in combination with linear combination of numerical atomic orbitals framework based density functional theory

Charge self-consistent dynamical mean field theory calculations in combination with linear combination of numerical atomic orbitals framework based density functional theory

Very high energy afterglow of structured jets: GW 170817 and prospects for future detections

We present a complete numerical model of the afterglow of a laterally structured relativistic ejecta from the radio to very high energies (VHE). This includes a self-consistent calculation of the synchrotron radiation, with its maximum frequency, and of synchrotron self-Compton (SSC) scattering that takes the Klein-Nishina regime into account. Attenuation due to pair production is also included. This model is computationally efficient and allows multi-wavelength data fitting. As a validation test, the radiative model was used to fit the broad-band spectrum of GRB 190114C at 90 s up to the TeV range. The full model was then used to fit the afterglow of GW 170817 and predict its VHE emission. We find that the SSC flux at the peak was much dimmer than the upper limit from H.E.S.S. observations. However, we show that either a smaller viewing angle or a higher external density would make similar off-axis events detectable in the future at VHE, even above 100 Mpc with the sensitivity of the Cherenkov telescope array. High external densities are expected in the case of fast mergers, but the existence of a formation channel for these binary neutron stars is still uncertain. We highlight that VHE afterglow detections would help to efficiently probe systems like this.

A Constraint-Based Orbital-Optimized Excited State Method (COOX).

In this work, we present a novel method to directly calculate targeted electronic excited states within a self-consistent field calculation based on constrained density functional theory (cDFT). The constraint is constructed from the static occupied-occupied and virtual-virtual parts of the excited state difference density from (simplified) linear-response time-dependent density functional theory calculations (LR-TDDFT). Our new method shows a stable convergence behavior, provides an accurate excited state density adhering to the Aufbau principle, and can be solved within a restricted SCF for singlet excitations to avoid spin contamination. This also allows the straightforward application of post-SCF electron-correlation methods like MP2 or direct RPA methods. We present the details of our constraint-based orbital-optimized excited state method (COOX) and compare it to similar schemes. The accuracy of excitation energies will be analyzed for a benchmark of systems, while the quality of the resulting excited state densities is investigated by evaluating excited state nuclear forces and excited state structure optimizations. We also investigate the performance of the proposed COOX method for long-range charge transfer excitations and conical intersections with the ground-state.

Insulating behaviour in room temperature rhombohedral LiNiO2 cathodes is driven by dynamic correlation

Abstract Inspired by the experimental finding of a paramagnetic insulating state in rhombohedral LiNiO2, a lithium-ion battery cathode of great interest, we calculate the electronic, magnetic, and optical properties of LiNiO2 employing a range of single-particle and many-body methods. Within density-functional theory (DFT) using the generalized-gradient approximation (GGA), meta-GGA, and hybrid functionals, we obtain a ferromagnetic half-metallic ground state for rhombohedral LiNiO2, as has been seen previously. Self-consistent GW calculations including self-interaction corrections beyond DFT for various flavours show an electronic band gap albeit with a small quasiparticle peak at the Fermi energy. Moving beyond this, room temperature state-of-the-art dynamical mean-field theory (DMFT) calculations on rhombohedral LiNiO2 show for the first time a gap of combined Mott and charge-transfer character. The paramagnetic insulating state has a band gap of ~0.6 eV, in excellent agreement with experiments and is in sharp contrast to DFT calculations that require the presence of an extra structural symmetry breaking in the form of Jahn–Teller distortions to open a gap. We observe Ni to be in a +2 state in a d 8L configuration, with a charge-transfer ligand hole in O p, and identify the ligand hole state from the DMFT DOS. We further show that whereas DFT shows the presence of an unphysical metallic Drude peak in the optical absorption spectra, DMFT calculations capture the correct form of the optical absorption spectra, and have an excellent match with the calculated band gap as well. Our results clarify that at room temperature, it is the charge transfer gap with a Mott character that causes rhombohedral LiNiO2’s insulating nature; a structural distortion is not required.

Quantifying spin-torque efficiency and magnetoresistance coefficient by microwave photoresistance in spin-torque ferromagnetic resonance

During the spin-torque ferromagnetic resonance (ST-FMR) measurement, the magnetization precession driven by the microwave field yields the radio frequency (rf) oscillating magnetoresistance and its time-averaged change (photoresistance). Here, we find that the strength of photoresistance can be directly determined by using dc bias current Idc modulating the symmetric component VS of the ST-FMR voltage spectrum. By measuring the angular dependence of photoresistance, we can quantify the in-plane and out-of-plane precession angles of ST-FMR, the actual rf current distribution in the magnetic and non-magnetic sublayers, and the magnitude of spin-torque and various magnetoresistance coefficients. These experimentally obtained values and analysis methods can more accurately quantify the spin-torque efficiency of both in-plane and out-of-plane spin polarizations by self-consistent calculation of the precession angle without harsh assumptions. And, we further confirm this universal method in three spintronic systems: the prototypical Pt/Py bilayer with anisotropic magnetoresistance (AMR), Py/Cu/Co20Tb80 spin valve trilayer with AMR and giant magnetoresistance, and [Co/Ni]3/Co/Pt multilayer with AMR and anisotropic interface magnetoresistance. This method eliminates potential deviation in calculating spin-torque efficiency by previously reported line shape analyzation and linewidth modulation methods of the ST-FMR technique and significantly extends its application range in characterizing spintronic materials and nanodevices.

Interaction-enhanced nesting in spin-fermion and Fermi-Hubbard models

The spin-fermion (SF) model postulates that the dominant coupling between low-energy fermions in near critical metals is mediated by collective spin fluctuations (paramagnons) peaked at the Néel wave vector, QN, connecting hot spots on opposite sides of the Fermi surface. It has been argued that strong correlations at hot spots lead to a Fermi surface deformation (FSD) featuring flat regions and increased nesting. This conjecture was confirmed in the perturbative self-consistent calculations when the paramagnon propagator dependence on momentum deviation from QN is given by χ−1∝|Δq|. Using diagrammatic Monte Carlo (diagMC) technique we show that such a dependence holds only at temperatures orders of magnitude smaller than any other energy scale in the problem, indicating that a different mechanism may be at play. Instead, we find that a χ−1∝|Δq|2 dependence yields a robust finite-T scenario for achieving FSD. To link phenomenological and microscopic descriptions, we applied the connected determinant diagMC method to the (t−t′) Hubbard model and found that at large U/t>5.5 before the formation of electron and hole pockets (i) the FSD defined as a maximum of the spectral function is not very pronounced; instead, it is the lines of zeros of the renormalized dispersion relation that deforms toward nesting, and (ii) the static spin susceptibility is well described by χ−1∝|Δq|2. Flat FS regions yield a nontrivial scenario for realizing a non-Fermi liquid state. Published by the American Physical Society 2024

Tensile test and finite element simulation of coarse-grained thin aluminium sheets

Abstract The aim of this work was to investigate the ability of finite element simulations applied to specimens containing only a few grains for tensile testing. For this purpose, two different finite element models were created: one with individual grains with individual flow curves generated by viscoplastic self-consistent (VPSC) calculations and one with uniform material properties throughout the cross-section of the sample. In comparison of the two models with experimental tensile tests, the following conclusions can be yielded. The measurement and the simulation with individual grains have the same deformation shape. Also, the mechanical properties (yield strength, tensile strength and elongation at break) were within 10% error. However, if the measurement results were compared to the simulation with homogeneous material, it showed an error up to 53%. Therefore, it can be stated that the tensile tests of these types of specimens can be simulated, but only if the grains are modelled individually.

Machine Learning for Predicting Ultralow Thermal Conductivity and High ZT in Complex Thermoelectric Materials.

Efficient and precise calculations of thermal transport properties and figures of merit, alongside a deep comprehension of thermal transport mechanisms, are essential for the practical utilization of advanced thermoelectric materials. In this study, we explore the microscopic processes governing thermal transport in the distinguished crystalline material Tl9SbTe6 by integrating a unified thermal transport theory with machine learning-assisted self-consistent phonon calculations. Leveraging machine learning potentials, we expedite the analysis of phonon energy shifts, higher-order scattering mechanisms, and thermal conductivity arising from various contributing factors, such as population and coherence channels. Our finding unveils an exceptionally low thermal conductivity of 0.31 W m-1 K-1 at room temperature, a result that closely correlates with experimental observations. Notably, we observe that the off-diagonal terms of heat flux operators play a significant role in shaping the overall lattice thermal conductivity of Tl9SbTe6, where the ultralow thermal conductivity resembles that of glass due to limited group velocities. Furthermore, we achieve a maximum ZT value of 3.17 in the c-axis orientation for p-type Tl9SbTe6 at 600 K and an optimal ZT value of 2.26 in the a-axis and b-axis direction for n-type Tl9SbTe6 at 500 K. The crystalline Tl9SbTe6 not only showcases remarkable thermal insulation but also demonstrates impressive electrical properties owing to the dual-degeneracy phenomenon within its valence band. These results not only elucidate the underlying reasons for the exceptional thermoelectric performance of Tl9SbTe6 but also suggest potential avenues for further experimental exploration.

Ab Initio Study of the Crystalline Structure of HgS under Low and High Pressure

This study analyzes the lattice dynamics of HgS under various pressures using ab initio self-consistent calculations based on the plane-wave method (PW) and generalized gradient approximation (GGA). The static study, performed by enthalpy calculations, predicts that the transition from the cinnabar phase (α-HgS) to the zinc-blende B3 (β-HgS) or wurtzite (2H) structures occurs at very low pressures, at 0.65 or 0.70 GPa, respectively. Furthermore, the transition from β-HgS to the rocksalt (B1) phase occurs at 7 GPa, and at high pressure, specifically at 110 GPa, HgS can adopt the CsCl (B2) phase. The mechanical study confirms the stability of the β and 2H phases at 0 GPa. Phonon calculations corroborate the results of the static and mechanical studies regarding stability (α→0.7GPa2H→0.9GPaβ), and the results indicate that the instabilities of the transverse acoustic (TA) modes, induced by the application of pressures of 10.5 GPa, 21 GPa, and 190 GPa, are responsible for the observed phase transitions in part of the Brillouin.

Tensor hypercontraction for fully self-consistent imaginary-time GF2 and GWSOX methods: Theory, implementation, and role of the Green's function second-order exchange for intermolecular interactions.

We present an efficient MPI-parallel algorithm and its implementation for evaluating the self-consistent correlated second-order exchange term (SOX), which is employed as a correction to the fully self-consistent GW scheme called scGWSOX (GW plus the SOX term iterated to achieve full Green's function self-consistency). Due to the application of the tensor hypercontraction (THC) in our computational procedure, the scaling of the evaluation of scGWSOX is reduced from O(nτnAO5) to O(nτN2nAO2). This fully MPI-parallel and THC-adapted approach enabled us to conduct the largest fully self-consistent scGWSOX calculations with over 1100 atomic orbitals with only negligible errors attributed to THC fitting. Utilizing our THC implementation for scGW, scGF2, and scGWSOX, we evaluated energies of intermolecular interactions. This approach allowed us to circumvent issues related to reference dependence and ambiguity in energy evaluation, which are common challenges in non-self-consistent calculations. We demonstrate that scGW exhibits a slight overbinding tendency for large systems, contrary to the underbinding observed with non-self-consistent RPA. Conversely, scGWSOX exhibits a slight underbinding tendency for such systems. This behavior is both physical and systematic and is caused by exclusion-principle violating diagrams or corresponding corrections. Our analysis elucidates the role played by these different diagrams, which is crucial for the construction of rigorous, accurate, and systematic methods. Finally, we explicitly show that all perturbative fully self-consistent Green's function methods are size-extensive and size-consistent.

Yu-Shiba-Rusinov States in s-Wave Kagome Superconductors: Self-Consistent Bogoliubov-de Gennes Calculations.

Significant research has recently been conducted into the Yu-Shiba-Rusinov (YSR) states in kagome superconductors through theoretical modeling and experimental investigations. However, additional efforts are still needed to further understand the local superconductivity near magnetic impurities in the kagome lattice and clarify how relevant quantities depend on the interaction strength, J, between such impurities and electrons. In this study, we explore a self-consistent numerical solution of the Bogoliubov-de Gennes equations for an s-wave superconducting Kagome model with a single classical magnetic impurity. Our study reveals that with increasing J, the local pair potential is systematically depressed in the vicinity of the impurity, similar to previous results obtained for the square and triangular lattices. Moreover, when J is further increased, the system undergoes a first-order phase transition with the appearance of stable and metastable states, reflecting the presence of the hysteresis loop in the pertinent quantities. As a consequence of this transition, the minimal energy of the stable YSR state is nonzero at any J, contrary to the expectations based on the assumption of a constant pair potential. A distinctive feature of the kagome lattice is that characteristics of the first-order transition are very sensitive to the position of the chemical potential within the kagome energy spectrum.

Decomposing Imaginary-Time Feynman Diagrams Using Separable Basis Functions: Anderson Impurity Model Strong-Coupling Expansion

We present a deterministic algorithm for the efficient evaluation of imaginary-time diagrams based on the recently introduced discrete Lehmann representation (DLR) of imaginary-time Green’s functions. In addition to the efficient discretization of diagrammatic integrals afforded by its approximation properties, the DLR basis is separable in imaginary-time, allowing us to decompose diagrams into linear combinations of nested sequences of one-dimensional products and convolutions. Focusing on the strong-coupling bold-line expansion of generalized Anderson impurity models, we show that our strategy reduces the computational complexity of evaluating an Mth-order diagram at inverse temperature β and spectral width ωmax from O((βωmax)2M−1) for a direct quadrature to O(M(log(βωmax))M+1), with controllable high-order accuracy. We benchmark our algorithm using third-order expansions for multiband impurity problems with off-diagonal hybridization and spin-orbit coupling, presenting comparisons with exact diagonalization and quantum Monte Carlo approaches. In particular, we perform a self-consistent dynamical mean-field theory calculation for a three-band Hubbard model with strong spin-orbit coupling representing a minimal model of Ca2RuO4, demonstrating the promise of the method for modeling realistic strongly correlated multiband materials. For both strong and weak coupling expansions of low and intermediate order, in which diagrams can be enumerated, our method provides an efficient, straightforward, and robust blackbox evaluation procedure. In this sense, it fills a gap between diagrammatic approximations of the lowest order, which are simple and inexpensive but inaccurate, and those based on Monte Carlo sampling of high-order diagrams. Published by the American Physical Society 2024

General Condition for Polymer Cononsolvency in Binary Mixed Solvents.

Starting from a generic model based on the thermodynamics of mixing and abstracted from the chemistry and microscopic details of solution components, three consistent and complementary computational approaches are deployed to investigate the general condition for polymer cononsolvency in binary mixed solvents at the zeroth order. The study reveals χPS - χPC + χSC as the underlying universal parameter that regulates cononsolvency, where χαβ is the immiscibility parameter between the α- and β-component. Two disparate cononsolvency regimes are identified for χPS - χPC + χSC < 0 and χPS - χPC + χSC > 2, respectively, based on the behavior of the second osmotic virial coefficient at varying solvent mixture composition x C. The predicted condition is verified using self-consistent field calculations by directly examining the polymer conformational transition as a function of x C. It is further shown that in the regime χPS - χPC + χSC < 0, the reentrant polymer conformation transition is driven by maximizing the solvent-cosolvent contact, but in the regime χPS - χPC + χSC > 2, it is driven by promoting polymer and cosolvent contact. In-between the two regimes when neither effect is dominant, a monotonic response of polymer conformation to x C is observed. Effects of the mean-field approximation on the predicted condition are evaluated by comparing the mean-field calculations with computer simulations. It shows that the fluctuation effects lead to a higher threshold value of χPS - χPC + χSC in the second regime, where local enrichment of cosolvent in polymer proximity plays a critical role.

On the ignition of H11B fusion fuel

We have revisited recent results on the ideal ignition of H11B fuel, in the light of the latest available reactivity, an alternative self-consistent calculation of the electron temperature, an increased extent of the suprathermal effects and the impact of plasma density. At high density, we find that the ideal ignition temperature is appreciably relaxed (e.g., Ti≃150 keV for ni∼1026 cm−3 and an optimal 11B/H concentration ε=0.15) and burn becomes substantial. We have then investigated central hot-spot ignition in both isobaric and isochoric inertial confinement configurations. Although implosion-driven ignition appears to be unfeasible, the isochoric self-heating conditions foster favourable preliminary conclusions on the utilization of proton fast ignition. In the isochoric case, we find a broad minimum in the ignition energy at ρR≃8.5 g/cm2 and 220≲Ti≲340 keV (80 ≲Te≲95 keV), for ε=0.15.

Carbon and Silicon Impurity Defects in GaN: Simulating Single-Photon Emitters by First Principles.

Defect single-photon emitters (SPE) in gallium nitride (GaN) have garnered great attentions in recent years due to the advantages they offer, including the ability to operate at room temperature, narrow emission linewidths, and high brightness. Nevertheless, the precise nature of the single-photon emission mechanism remains uncertain due to the multitude of potential defects that can form in GaN. In this work, our systematical investigation with the ab initio calculation indicates that carbon and silicon, as common dopants in gallium nitride, can interact with intrinsic defects in GaN and form new high-speed defect single-photon sources. Our findings identify a ternary defect NGaVNCN that possesses a short lifetime of less than 1 ns and a small zero-photon line (ZPL) of 864 nm. In other words, this defect can serve as a high-speed single photon source in the short wavelength window for fiber communication. In sharp contrast, the Si-supported defect NGaVNSiN has a higher unoccupied defect energy level which enters the conduction band and is therefore unsuitable for single photon emission. A systematic investigation has been conducted into the potential defects, thermal stability, and single-photon emission properties. The relaxation calculation and self-consistent calculations employed the Perdew-Burke-Ernzerhof exchange-correlation functional and Heyd-Scuseria-Ernzerhof exchange-correlation functional, respectively. These findings indicate the potential for high-performance single-photon sources through carbon or silicon doping of GaN.

Self-Consistent Calculations of Probabilities for the $${E}$$1 Transition between the Ground State and the $${[3_{1}^{-}\times 2_{1}^{+}]_{1^{-}}}$$ Two-Phonon State in Tin Isotopes

Self-Consistent Calculations of Probabilities for the $${E}$$1 Transition between the Ground State and the $${[3_{1}^{-}\times 2_{1}^{+}]_{1^{-}}}$$ Two-Phonon State in Tin Isotopes