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Seismology finds that Earth's solid inner core behaves anisotropically. Interpretation of this requires a knowledge of crystalline elastic anisotropy of its constituents-the major phase being most likely ε-Fe, stable only under high pressure. Here, single crystals of this phase are synthesized, and its full elasticity tensor is measured between 15 and 33 GPa at 300 K. It is calculated under the same conditions, using the combination of density functional theory and dynamical mean field theory, which describes explicitly electronic correlation effects. The predictive power of this scheme is checked by comparison with measurements; it is then used to evaluate the crystalline anisotropy in ε-Fe under higher density. This anisotropy remains of the same amplitude up to densities typical of Earth's inner core.

abinit is probably the first electronic-structure package to have been released under an open-source license about 20 years ago. It implements density functional theory, density-functional perturbation theory (DFPT), many-body perturbation theory (GW approximation and Bethe-Salpeter equation), and more specific or advanced formalisms, such as dynamical mean-field theory (DMFT) and the "temperature-dependent effective potential" approach for anharmonic effects. Relying on planewaves for the representation of wavefunctions, density, and other space-dependent quantities, with pseudopotentials or projector-augmented waves (PAWs), it is well suited for the study of periodic materials, although nanostructures and molecules can be treated with the supercell technique. The present article starts with a brief description of the project, a summary of the theories upon which abinit relies, and a list of the associated capabilities. It then focuses on selected capabilities that might not be present in the majority of electronic structure packages either among planewave codes or, in general, treatment of strongly correlated materials using DMFT; materials under finite electric fields; properties at nuclei (electric field gradient, Mössbauer shifts, and orbital magnetization); positron annihilation; Raman intensities and electro-optic effect; and DFPT calculations of response to strain perturbation (elastic constants and piezoelectricity), spatial dispersion (flexoelectricity), electronic mobility, temperature dependence of the gap, and spin-magnetic-field perturbation. The abinit DFPT implementation is very general, including systems with van der Waals interaction or with noncollinear magnetism. Community projects are also described: generation of pseudopotential and PAW datasets, high-throughput calculations (databases of phonon band structure, second-harmonic generation, and GW computations of bandgaps), and the library libpaw. abinit has strong links with many other software projects that are briefly mentioned.

We show that a calculation using density functional theory (DFT) in the generalized gradient approximation (GGA) supplemented by an explicit Coulomb interaction term between correlated electrons (GGA+U), can accurately describe structural properties of (1) the room temperature phases of U, Np, Pu, Am and Cm, and (2) the α, β, γ, δ and ϵ phases of plutonium, as does the combination of GGA with dynamical mean field theory (DMFT). It thus changes the view on the role of electronic interaction in these systems and opens the way to fast calculations of structural properties in actinides metallic system. We use ab initio values of effective Coulomb interactions and underline that Hund's exchange and spin-orbit coupling are of utmost importance in these calculations. Secondly, we show that phonons properties in δ plutonium are impacted by strong interactions. The GGA+DMFT results exhibits a lattice instability for the transverse (1 1 1) phonon mode. Moreover the amplitude of this lattice instability is consistent with the experimental temperature of stability of this phase. Our calculation thus shows that when the δ phase is thermodynamically unstable (at 0 K), it is also dynamically unstable.

We present a thermodynamical investigation of the α ⇌ γ transition of Ce using density functional theory within the projector augmented wave framework combined with the dynamical mean field theory. First, we confirm that without spin-orbit coupling no transition appears at zero temperature. Second, we extend the same conclusion to finite temperature with a slight difference: a crossover is observed both in temperature and pressure between the α and γ phases. This is obviously visible as a softening of the bulk modulus. Third, we show the leading role of entropy for the description of the equation of state of cerium. Last, we discuss the role of spin coupling, and we argue that neglecting the spin-orbit coupling is roughly equivalent to a renormalization of temperature. Indeed, at 800 K, both our variation of thermodynamical quantities and our spectral functions describe the experimental data. [ABSTRACT FROM AUTHOR]

Studying the anisotropic physical properties of hexagonal closed-packed (hcp) iron is essential for understanding the properties of the Earth’s inner core related to the preferred orientation of the inner core materials suggested by seismic observations. Investigating the anisotropic physical properties of hcp iron requires (1) the synthesis of hcp iron samples that exhibit several distinctive types of strong lattice preferred orientation (LPO) and (2) the quantitative LPO analysis of the samples. Here, we report the distinctive LPO of hcp iron produced from single-crystal body-centered cubic (bcc) iron compressed along three different crystallographic orientations ([100], [110], and [111]) in a diamond anvil cell based on synchrotron multiangle X-ray diffraction measurements up to 80 GPa and 300 K. The orientation relationships between hcp iron and bcc iron are consistent with the Burgers orientation relationship with variant selection. We show that the present method is a way to synthesize hcp iron with strong and characteristic LPO, which is beneficial for experimentally evaluating the anisotropic physical properties of hcp iron. [ABSTRACT FROM AUTHOR]

In this study, the structural, optical, and elastic properties of tetragonal MgTa2O6 and orthorhombic MgNb2O6 were determined using the Wien2k and ABINIT computational programs with the aid of density functional theory. The results imply that both compounds are classified as wide band gap semiconductor with 4.143 eV (for MgTa2O6) and 3.653 eV (for MgNb2O6) with PBEsol-GGA + TB-mBJ approximation. The findings of bulk modulus, shear modulus, Young modulus, Poisson's ratio, and anisotropy factors were determined and discussed in detail. The ductile behavior and the mechanism of structural stability were also explained. [ABSTRACT FROM AUTHOR]

Zirconium hydride is commonly used for next-generation reactor designs due to its excellent hydrogen retention capacity at temperatures below 1000 K. These types of reactors operate at thermal neutron energies and require accurate representation of thermal scattering laws (TSLs) to optimize moderator performance and evaluate the safety indicators for reactor design. In this work, we present an atomic-scale representation of sub-stoichiometric ZrH2−x (0.3 ≤ x ≤ 0.6) , which relies on ab initio molecular dynamics (AIMD) in tandem with velocity auto-correlation (VAC) analysis to generate phonon density of states (DOS) for TSL development. The novel NJOY+NCrystal tool, developed by the European Spallation Source community, was utilized to generate the TSL formulations in the A Compact ENDF (ACE) format for its utility in neutron transport software. First, stoichiometric zirconium hydride cross sections were benchmarked with experiments. Then sub-stoichiometric zirconium hydride TSLs were developed. Significant deviations were observed between the new δ -phase ZrH2−x TSLs and the TSLs in the current ENDF release. It was also observed that varying the hydrogen vacancy defect concentration and sites did not cause as significant a change in the TSLs (e.g., ZrH1.4 vs. ZrH1.7) as was caused by the lattice transformation from ϵ - to δ -phase. [ABSTRACT FROM AUTHOR]

An implementation of full self-consistency over the electronic density in the DFT + DMFT framework on the basis of a plane wave–projector augmented wave (PAW) DFT code is presented. It allows for an accurate calculation of the total energy in DFT + DMFT within a plane wave approach. In contrast to frameworks based on the maximally localized Wannier function, the method is easily applied to f electron systems, such as cerium, cerium oxide (Ce2O3) and plutonium oxide (Pu2O3). In order to have a correct and physical calculation of the energy terms, we find that the calculation of the self-consistent density is mandatory. The formalism is general and does not depend on the method used to solve the impurity model. Calculations are carried out within the Hubbard I approximation, which is fast to solve, and gives a good description of strongly correlated insulators. We compare the DFT + DMFT and DFT + U solutions, and underline the qualitative differences of their converged densities. We emphasize that in contrast to DFT + U, DFT + DMFT does not break the spin and orbital symmetry. As a consequence, DFT + DMFT implies, on top of a better physical description of correlated metals and insulators, a reduced occurrence of unphysical metastable solutions in correlated insulators in comparison to DFT + U.

The cerium γ⇄α transition was investigated using high-pressure, high-temperature angle-dispersive x-ray diffraction measurements on both poly- and single-crystalline samples, explicitly addressing symmetry change and transformation paths. The isomorphic hypothesis of the transition is confirmed, with a transition line ending at a solid-solid critical point. The critical exponent is determined, showing a universal behavior that can be pictured as a liquid-gas transition. We further report an isomorphic transition between two single crystals (with more than 14% of volume difference), an unparalleled observation in solid-state matter interpreted in terms of dislocation-induced diffusionless first-order phase transformation.

Recently, phonons with chirality (chiral phonons) have attracted significant attention. Chiral phonons exhibit angular and pseudoangular momenta. In circularly polarized Raman spectroscopy, the peak split of the Γ 3 mode is detectable along the principal axis of the chiral crystal in the backscattering configuration. In addition, peak splitting occurs when the pseudoangular momenta of the incident and scattered circularly polarized light are reversed. Until now, chiral phonons in binary crystals have been observed, whereas those in unary crystals have not been observed. Here, we observe chiral phonons in a chiral unary crystal Te. The pseudoangular momentum of the phonon is obtained in Te by an ab initio calculation. From this calculation, we verified the conservation law of pseudoangular momentum in Raman scattering. From this conservation law, we determined the handedness of the chiral crystals. We also evaluated the true chirality of the phonons using a measure with symmetry similar to that of an electric toroidal monopole., (© 2023 The Authors. Chirality published by Wiley Periodicals LLC.)

Understanding the origin of superconductivity in correlated two-dimensional materials is a key step in leveraging material engineering techniques for next-generation nanoscale devices. While it is widely accepted that phonons fluctuations only mediate conventional (s-wave) superconductivity, the common phenomenology of superconductivity in Bernal bilayer and rhombohedral trilayer graphene, as well as in a large family of graphene-based moiré systems, suggests a common superconducting mechanism across these platforms. In particular, in all these platforms some superconducting regions violate the Pauli limit, indicating unconventional superconductivity, naively ruling out conventional phonon-mediated pairing as the underlying mechanism. Here we combine first principles simulations with effective low-energy theories to investigate the superconducting mechanism and pairing symmetry in rhombohedral stacked graphene multilayers. We find that phonon-mediated superconductivity explains the main experimental findings, namely the displacement field and doping level dependence of the critical temperature, and the presence of two superconducting regions with different pairing symmetries that depend on the parent normal state. In particular, we find that intra-valley phonon scattering favors a triplet f-wave pairing when combined with electronic correlations stabilizing a spin- and valley-polarized normal state. We also propose a so far unexplored superconducting region at higher hole doping densities nh ≈ 4 × 1012 cm−2, and demonstrate how this highly hole-doped regime can be reached in heterostructures consisting of monolayer α-RuCl3 and rhombohedral trilayer graphene. Our findings promote phonon-mediated pairing as a strong contender to explain superconductivity across a wide range of graphene platforms, and demonstrate that phonons can, in fact, stabilize unconventional superconducting orders. [ABSTRACT FROM AUTHOR]

Magnetic materials can display many solutions to the electronic-structure problem, corresponding to different local or global minima of the energy functional. In Hartree-Fock or density-functional theory different single-determinant solutions lead to different magnetizations, ionic oxidation states, hybridizations, and inter-site magnetic couplings. The vast majority of these states can be fingerprinted through their projection on the atomic orbitals of the magnetic ions. We have devised an approach that provides an effective control over these occupation matrices, allowing us to systematically explore the landscape of the potential energy surface. We showcase the emergence of a complex zoology of self-consistent states; even more so when semi-local density-functional theory is augmented - and typically made more accurate - by Hubbard corrections. Such extensive explorations allow to robustly identify the ground state of magnetic systems, and to assess the accuracy (or not) of current functionals and approximations. [ABSTRACT FROM AUTHOR]

By using DFT simulations employing the GGA/PBE and LDA/CA-PZ approximations, the effects of the Hubbard U correction on the crystal structure, electronic properties, and chemical bands of the cubic phase (Pm3̅m) of STO were investigated. Our findings showed that the cubic phase (Pm3̅m) STO’s band gaps and lattice parameters/volume are in reasonably good accordance with the experimental data, supporting the accuracy of our model. By applying the DFT + U method, we were able to obtain band gaps that were in reasonably good agreement with the most widely used experimental band gaps of the cubic (Pm3̅m) phase of STO, which are 3.20 eV, 3.24 eV, and 3.25 eV. This proves that the Hubbard U correction can overcome the underestimation of the band gaps induced by both GGA/PBE and LDA/CA-PZ approximations. On the other hand, the Sr-O and Ti-O bindings appear predominantly ionic and covalent, respectively, based on the effective valence charges, electron density distribution, and partial density of states analyses. In an attempt to enhance the performance of STO for new applications, these results might also be utilized as theoretical guidance, benefitting from our precise predicted values of the gap energies of the cubic phase (Pm3̅m). [ABSTRACT FROM AUTHOR]

The linear combination of atomic orbitals (LCAO) method is advantageous for calculating important bulk and surface properties of crystals and defects in/on them. Compared to plane wave calculations and contrary to common assumptions, hybrid density functional theory (DFT) functionals are actually less costly and easier to implement in LCAO codes. However, choosing the proper basis set (BS) for the LCAO calculations representing Guassian-type functions is crucial, as the results depend heavily on its quality. In this study, we introduce a new basis set (BS) visual representation, which helps us (1) analyze the collective behavior of individual atoms' shell exponents (s, p, and d), (2) better compare different BSs, (3) identify atom-type invariant relationships, and (4) suggest a robust method for building a local all-electron BS (denoted as BS1) from scratch for each atom type. To compare our BS1 with the others existing in the literature, we calculate the basic bulk properties of SrTiO 3 (STO) in cubic and tetragonal phases using several hybrid DFT functionals (B3LYP, PBE0, and HSE06). After adjusting the exact Hartree–Fock (HF) exchange of PBEx, HSEx, and the state-of-the-art meta-GGA hybrid r 2 SCANx functionals, we find the r 2 SCAN15 and HSE27 for BS1, with the amount of exact HF exchange of 0.15 and 0.27, respectively, perform equally well for reproducing several most relevant STO properties. The proposed robust BS construction scheme has the advantage that all parameters of the obtained BS can be reoptimized for each new material, thus increasing the quality of DFT calculation predictions. [ABSTRACT FROM AUTHOR]

In the present study, we investigate the influence of boron (B) and phosphorus (P) (p- and n-type, respectively) doping on the electronic properties of ultra-thin silicon nanowires (SiNWs) by gradient-corrected density functional calculations with the Perdew–Burke–Ernzerhof (PBE) approximation. In the limit of very small diameters (5–8 Å), both pristine and highly active unsaturated SiNWs with orientations along the [001] and [111] directions exhibit electronic states around the Fermi level, indicative of conductive properties. Conduction is further enhanced by the introduction of doping atoms, as demonstrated by the relative change in the band structures of SiNWs with and without B and P doping. This investigation provides an important insight into the electronic states of SiNWs, which are candidates for future electronics or sensing applications. [ABSTRACT FROM AUTHOR]

Model Hamiltonians are regularly derived from first principles to describe correlated matter. However, the standard methods for this contain a number of largely unexplored approximations. For a strongly correlated impurity model system, here we carefully compare a standard downfolding technique with the best possible ground-truth estimates for charge-neutral excited-state energies and wave functions using state-of-the-art first-principles many-body wave function approaches. To this end, we use the vanadocene molecule and analyze all downfolding aspects, including the Hamiltonian form, target basis, double-counting correction, and Coulomb interaction screening models. We find that the choice of target-space basis functions emerges as a key factor for the quality of the downfolded results, while orbital-dependent double-counting corrections diminish the quality. Background screening of the Coulomb interaction matrix elements primarily affects crystal-field excitations. Our benchmark uncovers the relative importance of each downfolding step and offers insights into the potential accuracy of minimal downfolded model Hamiltonians. [ABSTRACT FROM AUTHOR]

In actinide systems, the 5 f electrons experience a uniquely delicate balance of effects and interactions having similar energy scales, which are often difficult to properly disentangle. This interplay of factors such as the dual nature of 5 f -states, strong electronic correlations, and strong spin–orbit coupling results in electronically unusual and intriguing behavior such as multi-k antiferromagnetic ordering, multipolar ordering, Mott-physics, mixed valence configurations, and more. Despite the inherent allure of their exotic properties, the exploratory science of even the more basic, binary systems like the actinide oxides has been limited due to their toxicity, radioactivity, and reactivity. In this article, we provide an overview of the available synthesis techniques for selected binary actinide oxides, including the actinide dioxides, sesquioxides, and a selection of higher oxides. For these oxides, we also review and evaluate the current state of knowledge of their crystal structures and magnetic properties. In many aspects, substantial knowledge gaps exist in the current body of research on actinide oxides related to understanding their electronic ground states. Bridging these gaps is vital for improving not only a fundamental understanding of these systems but also of future nuclear technologies. To this end, we note the experimental techniques and necessary future investigations which may aid in better elucidating the nature of these fascinating systems. [ABSTRACT FROM AUTHOR]

We emphasize, on the basis of experimental data and theoretical calculations, that the entropic stabilization of the gamma phase is the main driving force of the alpha-gamma transition of cerium in a wide temperature range below the critical point. Using a formulation of the total energy as a functional of the local density and of the f-orbital local Green's functions, we perform dynamical mean-field theory calculations within a new implementation based on the multiple linear muffin tin orbital (LMTO) method, which allows us to include semicore states. Our results are consistent with the experimental energy differences and with the qualitative picture of an entropy-driven transition, while also confirming the appearance of a stabilization energy of the alpha phase as the quasiparticle Kondo resonance develops.

Heterostructure engineering is an effective technology to improve photo-electronic properties of two dimensional layered semiconductors. In this paper, based on first principles method, we studied the structure, stability, energy band, and optical properties of ZnSe/SnSe heterostructure change with film layer. Results show that all heterostructures are the type-II band arrangement, and the interlayer interaction is characterized by van der Waals. The electron concentration and charge density difference implies the electron (holes) transition from SnSe to monolayer ZnSe. By increasing the layer of SnSe films, the quantum effects are weakened leading to the band gap reduced, and eventually show metal properties. The optical properties also have obvious change, the excellent absorption ability of ZnSe/SnSe heterostructures mainly near the infrared spectroscopy. These works suggest that ZnSe/SnSe heterostructure has significant potential for future optoelectronic applications. [ABSTRACT FROM AUTHOR]

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Polarons and spin-orbit (SO) coupling are distinct quantum effects that play a critical role in charge transport and spin-orbitronics. Polarons originate from strong electron-phonon interaction and are ubiquitous in polarizable materials featuring electron localization, in particular 3d transition metal oxides (TMOs). On the other hand, the relativistic coupling between the spin and orbital angular momentum is notable in lattices with heavy atoms and develops in 5d TMOs, where electrons are spatially delocalized. Here we combine ab initio calculations and magnetic measurements to show that these two seemingly mutually exclusive interactions are entangled in the electron-doped SO-coupled Mott insulator Ba2Na1−xCaxOsO6 (0 < x < 1), unveiling the formation of spin-orbital bipolarons. Polaron charge trapping, favoured by the Jahn-Teller lattice activity, converts the Os 5d1 spin-orbital Jeff = 3/2 levels, characteristic of the parent compound Ba2NaOsO6 (BNOO), into a bipolaron 5d2 Jeff = 2 manifold, leading to the coexistence of different J-effective states in a single-phase material. The gradual increase of bipolarons with increasing doping creates robust in-gap states that prevents the transition to a metal phase even at ultrahigh doping, thus preserving the Mott gap across the entire doping range from d1 BNOO to d2 Ba2CaOsO6 (BCOO).The interplay between electron-phonon and spin-orbit interactions has led to the concept of a spin-orbit polaron. Here the authors show that such a regime is realized in a spin-orbit-coupled Mott insulator, leading to a new polaron quasiparticle, and study its effect on the Mott metal-insulator transition. [ABSTRACT FROM AUTHOR]

The quest for novel materials with extraordinary electronic and plasmonic properties is an ongoing pursuit in the field of materials science. The dataset provides the results of a computational study that used ab initio and semi-analytical computations to model freestanding nanosystems. We delve into the world of ribbon-like materials, specifically graphene nanoribbons, silicene nanoribbons, and germanene nanoribbons, comparing their electronic and plasmonic characteristics. Our research reveals a myriad of insights, from the tunability of band structures and the influence of an atomic number on electronic properties to the adaptability of nanoribbons for optoelectronic applications. Further, we uncover the promise of these materials for biosensing, demonstrating their plasmon frequency tunability based on charge density and Fermi velocity modification. Our findings not only expand the understanding of these quasi-1D materials but also open new avenues for the development of cutting-edge devices and technologies. This data presentation holds immense potential for future advancements in electronics, optics, and molecular sensing. Dataset:  https://doi.org/10.17605/OSF.IO/BMUSV Dataset License: CC-BY-4.0 [ABSTRACT FROM AUTHOR]

As UO2 is easily oxidized during the nuclear fuel cycle it is important to have a detailed understanding of the structures and properties of the oxidation products. Experimental work over the years has revealed many stable uranium oxides including UO2, U4O9 (UO2.25), U3O7 (UO2.33), U2O5 (UO2.5), U3O8 (UO2.67), and UO3, all with a number of different polymorphs. These oxides are broadly split into two categories, fluorite-based structures with stoichiometries in the range of UO2 to UO2.5 and less dense layered-type structures with stoichiometries in the range of UO2.5 to UO3. While UO2 is well characterized, both experimentally and computationally, there is a paucity of data concerning higher stoichiometry oxides in the literature. In this work we determine the ambient melting points of all the six stoichiometric uranium oxides listed above and compare them to the available experimental and/or theoretical data. We demonstrate that a family of the six ambient melting points map out a solid-liquid transition boundary consistent with the high-temperature portion of the phase diagram of uranium-oxygen system suggested by Babelot et al. [ABSTRACT FROM AUTHOR]

Metal matrix composites have attracted extensive attention from both the research and industrial perspective. In this study, we prepared aluminum-reduced graphene oxide (Al–rGO) composites with enhanced thermal conductivity in an easy single-step process. Pristine Al shows a thermal conductivity of 175 Wm−1K−1 (standard deviation <5%), which increases to 293 Wm−1K−1 for an Al–rGO composite with 1% rGO. Analysis of theoretical models shows that a higher percentage of rGO inside the Al matrix creates a continuous network resulting in more available phase space through which heat carrier phonons travel with less scattering, and hence thermal conductivity of the composite increases. Furthermore, Al–rGO composites show an ∼5% increase in microhardness compared with pristine Al. The electrical resistivity of the composite is comparable to that of pristine Al for a narrow weight percentage of rGO, whereas a 70% enhancement in the thermal conductivity of the composite is observed for the same weight percentage range, suggesting possibilities for exploiting both high electrical and thermal conductivities for various applications. [ABSTRACT FROM AUTHOR]