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DOE OSTI2026

A comprehensive first-principles study of the effects of the exchange-correlation functional and magnetism on defect and diffusion properties of the CoCrNi medium-entropy alloy

The present work is a novel, systematic study of the effect of density functional theory input parameters on the vacancy formation energy (VFE), migration barrier for diffusion, and electronic structure for each element in the CoCrNi medium-entropy alloy (MEA). In particular, the novelties include: (1) calculating the aforementioned properties of Co, Cr, or Ni, in the CoCrNi MEA using magnetic and non-magnetic states, and two versions of the generalized gradient approximation: Perdew, Burke, and Ernzerhof (PBE) and the PBE version for solids (PBEsol), and (2) a detailed comparison of 0 K activation energy to experimental creep activation energies. First-principles calculations at 0 K are performed using the Vienna ab-initio simulation package. Special quasirandom structures (SQS) and Widom-type substitution are employed. For each element, Co, Cr, or Ni, non-magnetic calculations result in a higher VFE and larger range of calculated values for the configurations studied. The averaged migration barrier is the highest for Co in the CoCrNi for three of four sets of calculation parameters in the configurations studied. Finally, the results indicate that the average 0 K activation energy for diffusion makes up 70–80% of the experimental creep activation energy, depending on the exchange-correlation functional employed.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Assessing the Limitations of Self-Interaction-Corrected Functionals for Describing the Hydrated Electron

Simulating the hydrated electron using density functional theory is challenging due to the prevalence of self-interaction error in standard functionals. Hybrid functionals like PBEh(40) can reasonably describe the chemistry of an excess electron in water and partially mitigate self-interaction error by incorporating exact Hartree–Fock exchange, but they are computationally expensive making them impractical for large-scale and long-time ab initio molecular dynamics simulations. Explicit self-interaction correction schemes that are applied on an orbital-by-orbital basis offer a potential alternative when the correction is limited to the singly occupied molecular orbital obtained with a generalized gradient approximation functional. Here, we examine whether the Perdew–Zunger self-interaction correction scheme applied to the revPBE functional can provide a computationally efficient and physically sensible alternative to PBEh(40) for the hydrated electron. We find that functionals incorporating a self-interaction correction scheme should be viewed with caution when applied to the hydrated electron and its reactivity. Furthermore, we show that it is critical to consider extensive sampling and diverse chemical environments when validating their performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Lattice Structure and Dynamics of Sparse Molecular Crystals: OsO 4 and RuO 4

OsO 4 and RuO 4 are molecular oxides with unique tetrameric structures and rare +8 oxidation states. Accurately modeling their properties remains challenging for density functional theory (DFT) due to weak intertetramer interactions, which standard functionals fail to capture. Here, in this work, we show that the van der Waals (vdW)-corrected density functional (vdW-DF-optB86b) provides structural parameters that are much closer to experimental values than the standard generalized gradient approximation, with volume predictions that fall within the experimentally observed range. Phonon band structure analysis shows that the inclusion of vdW interactions stabilizes soft phonon modes, highlighting the importance of dispersion corrections for accurate predictions of lattice dynamics. Experimental measurements of the phonon density of states for OsO 4 , obtained via inelastic neutron scattering, demonstrate good agreement with our vdW-DF-optB86b calculations. These results validate OsO 4 and RuO 4 as valuable benchmarks for structural and vibrational calculations via vdW-corrected DFT methods and offer insights for studying the broader class of sparse molecular materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Efficient simulations of charge density waves in the transition metal Dichalcogenide TiSe 2

Charge density waves (CDWs) in transition metal dichalcogenides are the subject of growing scientific interest due to their rich interplay with exotic phases of matter and their potential technological applications. Here, using density functional theory with advanced meta-generalized gradient approximations (meta-GGAs) and linear response time-dependent density functional theory (TDDFT) with state-of-the-art exchange-correlation kernels, we investigate the electronic, vibrational, and optical properties in 1T-TiSe 2 with and without CDW. In both bulk and monolayer TiSe 2 , the electronic bands and phonon dispersions in either normal or CDW (semiconducting) phase are described well via meta-GGAs, which separate the valence and conduction bands just as HSE06 does but with significantly more computational feasibility. The experimentally observed humps of electron energy loss spectroscopy are successfully reproduced in TDDFT. Our work opens the door to simulating these complexities in CDW compounds from first principles by revealing meta-GGAs as an accurate low-cost alternative to HSE06.

Electronic properties and materials↗

DOE OSTI2025

MP-ALOE: an r2SCAN dataset for universal machine learning interatomic potentials

We present MP-ALOE, a dataset of nearly 1 million DFT calculations using the accurate r2SCAN meta-generalized gradient approximation. Covering 89 elements, MP-ALOE was created using active learning and primarily consists of off-equilibrium structures. We benchmark a machine learning interatomic potential trained on MP-ALOE, and evaluate its performance on a series of benchmarks, including predicting the thermochemical properties of equilibrium structures; predicting forces of far-from-equilibrium structures; maintaining physical soundness under static extreme deformations; and molecular dynamic stability under extreme temperatures and pressures. MP-ALOE shows strong performance on all of these benchmarks and is made public for the broader community to utilize.

Kuner, Matthew C↗

DOE OSTI2025

Optical properties of BaTiO 3 at room temperature: DFT modelling

The optical properties of the tetragonal phase of BaTiO 3 have been studied using density functional methods, applying the generalized gradient approximation at room temperature and a hybrid functional for static lattice analysis.

Chemistry↗

DOE OSTI2026

Mott vs Kondo: Influence of various density functional based methods on the Ce isostructural phase transition mechanism

The cerium iso-structural phase transition (γ–α) is dominated by f-electron localization changes that results in a magnetic ordering change and a volume collapse. Generally, these physics are difficult to capture with ab initio and first principles methods. However, previous works have shown various methods to be successful in predicting at least some of the physics of the γ to α phase transition. Therefore, here, we perform a broad survey of density functional based methods across three levels of theory and types of functions [GGA (generalized gradient approximation), MetaGGA, and hybrid functionals] and compare the results, focusing on hydrostatic compression across the phase boundary at zero kelvin. For the methods that best reproduce experimental results, we directly probe the predicted mechanisms and frame the results in the Mott/Kondo debate, assessing how the underlying methods and assumptions of different functionals can assess the physical drivers in the phase transition, providing insight into the governing processes of this unique phase transition.

36 MATERIALS SCIENCE↗

DOE OSTI2025

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↗

DOE OSTI2026

Electronic transport, thermal transport, thermal expansion, and magnetization in the strongly correlated metal LaNi⁢O 3

Perovskite structured LaNiO 3 is a strongly correlated metal with intriguing thermal and magnetic properties. The volume dependence of calculated and measured physical properties can add additional critical information to develop a more in-depth understanding of this strongly correlated phenomenon. Taking advantage of recent single crystal LaNiO 3 growth using the floating-zone method, we have measured the thermal expansion, the magnetostriction, and the pressure dependence of the magnetic susceptibility, which then allows derivation of the Grüneisen parameters γ e = $\frac{dlnN(E_F)}{d lnV}$, γ χ = $\frac{dlnχ}{d lnV}$, as well as of electric and thermal transport properties. We simulate the volume dependence of structural and magnetic properties using Density Functional Theory calculations at the Generalized Gradient Approximation level. A large discrepancy between experimental values and calculated ones suggests that strong correlations are likely to be dynamic in nature. This study also provides a side-by-side comparison of measurements in single crystal and polycrystalline samples of LaNiO 3 to elucidate intrinsic materials properties. A broad hump at high temperatures in the temperature dependence of magnetization found in the single crystal sample of LaNiO 3 has been rationalized by a model that includes the influence of electron correlations on the Landau diamagnetism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

Anomalous elastic softening in ferroelectric hafnia under pressure

his study employs first-principles density-functional theory (DFT) calculations to explore the elastic and mechanical properties of ferroelectric hafnia (HfO 2 ) in its polar orthorhombic 𝑃⁢𝑐⁢𝑎⁢2 1 phase under varying hydrostatic pressure conditions up to 30 GPa. Utilizing a plane-wave basis set and Perdew-Burke-Ernzerhof generalized-gradient approximation for solids in our DFT calculations, we investigate both pure and yttrium-substituted HfO 2 . Our findings reveal an anomalous reduction in the 𝐶 33 component of the elastic tensor with increasing pressure, which becomes significant above 15 GPa and signals a potential pressure-driven structural phase transition at higher pressure. The analysis of atomic displacements under pressure sheds light on the unusual mechanical behavior and phase stability of this material. Additionally, we observe a transition from an indirect band gap to a direct band gap with increasing pressure, which could have significant implications for optical applications. Here, the effects of yttrium substitution on the mechanical and electronic properties are further examined, revealing that yttrium substitution softens the elastic response of this material and reduces the electronic band gap. These results enhance our understanding of elastic and mechanical responses of ferroelectric hafnia and its potential for applications in microelectronics, piezoelectric devices, and nonvolatile ferroelectric random-access memories. Further experimental validation is recommended to confirm our predictions and explore the practical implications of the observed phase transitions and electronic behavior of the ferroelectric hafnia under high-pressure conditions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Exploring interlayer coupling in the twisted bilayer PtTe 2

We have investigated interlayer interactions in the bilayer PtTe 2 system, which influence the electronic energy bands near the Fermi level. Our diffusion Monte Carlo (DMC) calculations for the high-symmetry bilayer stackings (AA, AB, AC) manifest distinct interlayer binding characteristics among the stacking modes by revealing significantly different interlayer separations depending on the stacking, which is critical to understanding the interlayer coupling of the twisted bilayers consisting of various local stacking arrangements. Furthermore, a comparison between the interlayer separations obtained from DMC and density functional theory (DFT) shows that meta-generalized gradient approximation (GGA)-based van der Waals–DFT results agree with DMC for different layer stackings, including twisted bilayers, but only the ground-state AA stacking matches well with GGA-based DFT predictions. This underscores the importance of accurate exchange-correlation potentials even for capturing the stacking-dependent interlayer binding properties. We further show that the variability in DFT-predicted interlayer separations is responsible for the large discrepancy of band structures in the 21 . 79 ∘ twisted bilayer PtTe 2 , affecting its classification as metallic or insulating. These results demonstrate the importance of obtaining a correct description of stacking-dependent interlayer coupling in modeling delicate bilayer systems at finite twists. Published by the American Physical Society 2024

36 MATERIALS SCIENCE↗

DOE OSTI2025

Range-separated thermal hybrid exchange-correlation density functional for accurate band-gap calculations of warm dense matter

Here, in this study, we present a range-separated thermal hybrid exchange-correlation (XC) functional, termed RS-KDT0, which provides highly accurate band-gap predictions at elevated temperature while reducing the computational cost relative to thermal global hybrid functionals. At zero temperature, RS-KDT0 recovers the widely used ground-state range-separated hybrid functional HSE06. To assess its performance across temperature regimes, we conducted static calculations of electronic pressure, band gaps, and band structures. RS-KDT0 exhibits the same level of accuracy as HSE06 in the low-temperature regime and demonstrates improved agreement with finite-temperature GW calculations at elevated temperatures when compared to other thermal XC functionals such as the generalized gradient approximation (GGA)-level KDT16 and the global hybrid KDT0.

density functional theory↗

NASA NTRS1987

Approximate polynomial preconditioning applied to biharmonic equations on vector supercomputers

Applying a finite difference approximation to a biharmonic equation results in a very ill-conditioned system of equations. This paper examines the conjugate gradient method used in conjunction with the generalized and approximate polynomial preconditionings for solving such linear systems. An approximate polynomial preconditioning is introduced, and is shown to be more efficient than the generalized polynomial preconditionings. This new technique provides a simple but effective preconditioning polynomial, which is based on another coefficient matrix rather than the original matrix operator as commonly used.

Wong, Yau Shu↗

NASA NTRS1983

Structural optimization - Challenges and opportunities

A review of developments in structural optimization techniques and their interface with growing computer capabilities is presented. Structural design steps comprise functional definition of an object, an evaluation phase wherein external influences are quantified, selection of the design concept, material, object geometry, and the internal layout, and quantification of the physical characteristics. Optimization of a fully stressed design is facilitated by use of nonlinear mathematical programming which permits automated definition of the physics of a problem. Design iterations terminate when convergence is acquired between mathematical and physical criteria. A constrained minimum algorithm has been formulated using an Augmented Lagrangian approach and a generalized reduced gradient to obtain fast convergence. Various approximation techniques are mentioned. The synergistic application of all the methods surveyed requires multidisciplinary teamwork during a design effort.

Sobieszczanski-Sobieski, J.↗

NASA NTRS1984

Structural optimization: Challenges and opportunities

Sobieszczanski-Sobieski, J.↗

NASA NTRS1972

Effects of gravity-gradient torque on the rotational motion of a triaxial satellite in a precessing elliptic orbit.

A method of general perturbations, based on the use of Lie series to generate approximate canonical transformations, is applied to study the effects of gravity-gradient torque on the rotational motion of a triaxial, rigid satellite. The center of mass of the satellite is constrained to move in an elliptic orbit about an attracting point mass. The orbit, which has a constant inclination, is free to precess and spin. The method of general perturbations is used to obtain the Hamiltonian for the nonresonant secular and long-period rotational motion of the satellite. The differential equations derivable from the transformed Hamiltonian are integrable, and the solution for the long-term motion may be expressed in terms of Jacobian elliptic functions and elliptic integrals. Geometrical aspects of the long-term rotational motion are discussed, and a comparison of theoretical results with observations is made.

Cochran, J. E.↗

NASA NTRS2003

The Galileo Probe: How it Has Changed Our Understanding of Jupiter

The Galileo Mission to Jupiter, which arrived in December of 1995, provided the first study by an orbiter, and the first in-situ sampling via an entry probe, of an outer planet atmosphere. The rationale for an entry probe is that, even from an orbiter, remote sensing of the jovian atmosphere could not adequately retrieve the information desired. This paper provides a current summary of the most significant aspects of the data returned from the Galileo entry probe. As a result of the probe measurements, there has been a reassessment of our understanding of outer planet formation and evolution of the solar system. The primary scientific objective of the Galileo probe was to determine the composition of the jovian atmosphere, which from remote sensing remained either very uncertain, or completely unknown, with respect to several key elements. The probe found that the global He mass fraction is. significantly above the value reported from the Voyager Jupiter flybys but is slightly below the protosolar value, implying that there has been some settling of He to the deep jovian interior. The probe He measurements have also led to a reevaluation of the Voyager He mass fraction for Saturn, which is now determined to be much closer to that of Jupiter. The elements C, N, S, Ar, Kr, Xe were all found to have global abundances approximately 3 times their respective solar abundances. This result has raised a number of fundamental issues with regard to properties of planetesimals and the solar nebula at the time of giant planet formation. Ne, on the other hand, was found to be highly depleted, probably as the result of it being carried along with helium as helium settles towards the deep interior. The global abundance of O was not obtained by the probe because of the influence of local processes at the probe entry site (PES), processes which depleted condensible species, in this case H2O, well below condensation levels. Other condensible species, namely NH3 and H2S, were similarly affected but attained their deep equilibrium mixing ratios before the maximum depth sampled by the probe. Processes that might be capable of producing such effects on the condensibles are still under investigation. Measured isotopic ratios of noble gases and other heavy elements are solar, and (D + (Sup 3)He)/H is the same to within measurement uncertainties as in the local interstellar medium. No thick clouds were detected, and in particular no significant water cloud, but the PES location clearly affected the probe measurements of clouds. In fact, the probe data must be understood in the context of the location of the PES, which was within what is termed a 5 micron hot spot, a local clearing in the clouds that is bright near the 5 microns spectral region. The thermal structure at the PES was determined from approximately 1000 km above the 1 bar pressure level (10(exp -9 bars)) to 132 km 1 bar (22bars). The probe showed the atmosphere to have a generally sub-adiabatic temperature gradient (static stability) of = 0.1 K/km to as deep as the probe made measurements. In the upper atmosphere the probe derived a maximum positive vertical temperature gradient of approximately 5 K/km, and maximum temperature of = 900 K. The energy sources producing the warm upper atmosphere have yet to be completely identified. At first glance, Doppler tracking of the probe indicates that the long observed cloud level zonal winds extend to levels at least as deep as the probe made measurements. Zonal wind increases from = 80 m/s at pressures less than a bar to about 180 m/s near 5 bars, and remains approximately constant with depth thereafter. However, there is a question as to whether the winds measured from probe tracking are representative of the general wind field, or are considerably influenced by localized winds associated with the PES.

Young, Richard E.↗

NASA NTRS2008

Comparative In Situ Measurements of Plasma Instabilities in the Equatorial and Auroral Electrojets

This presentation provides a comparison of in situ measurements of plasma instabilities gathered by rocket-borne probes in the equatorial and auroral electrojets. Specifically, using detailed measurements of the DC electric fields, current density, and plasma number density within the unstable daytime equatorial electrojet from Brazil (Guara Campaign) and in the auroral electrojet from Sweden (ERRIS Campaign), we present comparative observations and general conclusions regarding the observed physical properties of Farley-Buneman two-stream waves and large scale, gradient drift waves. The two stream observations reveal coherent-like waves propagating near the E x B direction but at reduced speeds (nearer to the presumed acoustic velocity) with wavelengths of approximately 5-10m in both the equatorial and auroral electrojet, as measured using the spaced-receiver technique. The auroral electrojet data generally shows extensions to shorter wavelengths, in concert with the fact that these waves are driven harder. With respect to gradient-drift driven waves, observations of this instability are much more pronounced in the equatorial electrojet, given the more favorable geometry for growth provided by the vertical gradient and horizontal magnetic field lines. We present new analysis of Guara rocket observations of electric field and plasma density data that reveal considerable structuring in the middle and lower portion of the electrojet (90-105 km) where the ambient plasma density gradient is unstable. Although the electric field amplitudes are largest (approximately 10-15 mV/m) in the zonal direction, considerable structure (approximately 5-10 mV/m) is also observed in the vertical electric field component as well, implying that the dominant large scale waves involve significant vertical interaction and coupling within the narrow altitude range where they are observed. Furthermore, a detailed examination of the phase of the waveforms show that on some, but not all occasions, locally enhanced eastward fields are associated with locally enhanced upwards (polarization) electric fields. The measurements are discussed in terms of theories involving the non-linear evolution and structuring of plasma waves.

Pfaff, Robert F.↗