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159 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Isostructural Phase Transition of Fe 2 ⁢O 3 under Laser Shock Compression

We present in situ x-ray diffraction and velocity measurements of Fe 2⁢ O 3 under laser shock compression at pressures between 38–122 GPa. None of the high-pressure phases reported by static compression studies were observed. Instead, we observed an isostructural phase transition from 𝛼−Fe 2⁢ O 3 to a new 𝛼′−Fe 2 ⁢O 3 phase at a pressure of 50–62 GPa. The 𝛼′−Fe 2⁢ O 3 phase differs from 𝛼−Fe 2 ⁢O 3 by an 11% volume drop and a different unit cell compressibility. We further observed a two-wave structure in the velocity profile, which can be related to an intermediate regime where both 𝛼 and 𝛼′ phases coexist. Furthermore, density functional theory calculations with a Hubbard parameter indicate that the observed unit cell volume drop can be associated with a spin transition following a magnetic collapse.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Direct time-domain determination of electron-phonon coupling strengths in chromium

In this work, we report the results of an ultrafast, direct structural measurement of optically pumped phonons in a Cr thin film using ultrashort x-ray pulses from a free-electron laser. In addition to measuring and confirming the known long-wavelength dispersion relation of Cr along a particular acoustic branch, we are able to determine the relative phase of the phonons as they are generated. The Cr sample exhibits two generation mechanisms for the phonons: the releasing of a preexisting charge density wave at higher frequencies, and the creation of an acoustic strain pulse via laser heating that dominates at lower frequencies. Furthermore, for the latter mechanism, we are able to measure the frequency dependence of the time required to generate the phonons. To explain the observed magnitude and slope of the delays, we perform first-principles simulations in the framework of density functional perturbation theory and ab initio molecular dynamics to fit anharmonic phonon models. In conclusion, these results show that the wave-vector dependence of the electron-phonon coupling is the driving mechanism behind the delay times: Phase-space limitation leads to higher times near the zone center. The absolute magnitudes of the delay times measured are found to be much shorter than the equilibrium electron-phonon coupling times we compute, indicating that the coupling strength is greatly enhanced when the electronic system is out of equilibrium with the lattice, as has been seen in bismuth and other systems.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Discovery of Stacking Heterogeneity, Layer Buckling, and Residual Water in COF-999-NH 2 and Implications on CO 2 Capture

Covalent organic frameworks (COFs), with their modular architectures and tunable functionalities, provide a versatile platform to design sorbents for the direct capture of CO 2 from air. Here, for this work, we combined density functional theory, molecular dynamics, and grand canonical Monte Carlo simulations with experiment to understand structural factors for furthering COF-999-NH 2 ’s performance as the precursor to COF-999 for direct air CO 2 capture. Small energy differences among laterally shifted stackings suggest intrinsic stacking heterogeneity. The simulations show pronounced layer buckling coupled to extensive amine–nitrile hydrogen bonding and persistent pore water, which initiates undesired polymerization and undermines uptake. The predicted presence of water is confirmed by subsequent experiments. These insights point to a single, actionable design rule: exclude retained water by introducing hydrophobic pore environments to maximize the CO 2 capture efficiency.

adsorption↗
DOE OSTI2026

Machine learning-based interatomic potential development and phase transition analysis of ferroelectric hafnium dioxide

The ferroelectric phase (𝑃⁢𝑐⁢𝑎⁢2 1 , which is in orthorhombic symmetry) of hafnium dioxide (HfO 2 ) has gained much attention due to its potential applications in nanoelectronics and advanced memory devices. However, its complex phase behavior under external stimuli, such as pressure and temperature, remains a subject of intense investigation. This study focuses on developing a machine learning-based interatomic potential (MLIP) that is trained with data from density-functional theory (DFT) calculations to simulate phase transitions and mechanical properties of HfO 2 . The developed MLIP predicts lattice parameters, equations of state, bulk and shear moduli, and elastic constants that closely align with DFT predictions for several phases and at various pressures. Once validated, the MLIP is used to investigate the phase transitions of ferroelectric HfO 2 (𝑃⁢𝑐⁢𝑎⁢2 1 ) under both isobaric and constant stress conditions at elevated temperatures ranging from 200 to 2500 K. We used several complementary methods, including local symmetry identification, radial distribution function, and x-ray diffraction characterization, to identify interesting phase transitions among several competitive hafnia phases predicted from our simulations. The suggested methods uniformly reveal that under pure deviatoric condition, the system favors a transition from the orthorhombic 𝑃⁢𝑐⁢𝑎⁢2 1 phase to a tetragonal (𝑃⁢4 2 /𝑛⁢𝑚⁢𝑐) phase, whereas a zero stress condition drives the system from the 𝑃⁢𝑐⁢𝑎⁢2 1 phase to another orthorhombic (𝑃⁢𝑏⁢𝑐⁢𝑛) phase. These findings provide crucial insights into stress and temperature-induced phase behavior of hafnia, guiding future experimental and theoretical studies for optimizing hafnia-based ferroelectric devices.

Ferroelectric HfO2↗
DOE OSTI2026

3⁢𝑄 magnetic order with spatially alternating spin scalar chirality in overdoped C⁢o 0.336⁢ Ta⁢S 2

C⁢o 𝑥 ⁢Ta⁢S 2 (𝑥≈1/3) exhibits a spontaneous Hall effect from spin texture in antiferromagnets, with a tetrahedral triple-Q (3Q) order and uniform spin scalar chirality. Upon Co overdoping (𝑥>1/3), it undergoes a shift in magnetic ordering vectors from 𝐐 m =(1/2, 0, 0) to (1/3, 0, 0). Interestingly, the spontaneous Hall effect disappeared in the overdoped regime, which was originally attributed to the loss of 3Q order. However, a question remains whether a new type of 3Q order can exist with alternating chirality in the overdoped regime. To address this, we investigated C⁢o 0.336⁢ Ta⁢S 2 using inelastic neutron scattering (INS), neutron diffraction, and optical dichroism, and found that INS data and spin-wave simulations support a 3Q order with alternating chirality. Moreover, neutron diffraction data show field-independent Bragg peaks, while linear dichroism detects no in-plane anisotropy, consistent with threefold rotation symmetry. Our data support the scenario of an alternating-chirality 3Q order in C⁢o 0.336 ⁢Ta⁢S 2 , canceling the spontaneous Hall effect. Furthermore, this study highlights a combined neutron-optical approach to identify complex spin textures.

Landau-Lifschitz-Gilbert equation↗
DOE OSTI2023

Static and dynamical properties of the spin-$\frac{5}{2}$ nearly ideal triangular lattice antiferromagnet $\mathrm{Ba_3}$ $\mathrm{MnSb_2}$ $\mathrm{O_9}$

Here, we study the ground state and spin excitations in Ba 3 MnSb 2 O 9 , an easy-plane S = 5/2 triangular lattice antiferromagnet. By combining single-crystal neutron scattering, electric spin resonance (ESR), and spin wave calculations, we determine the frustrated quasi-two-dimensional spin Hamiltonian parameters describing the material. While the material has a slight monoclinic structural distortion, which could allow for isosceles-triangular exchanges and biaxial anisotropy by symmetry, we observe no deviation from the behavior expected for spin waves in the in-plane $120$° state. Even the easy-plane anisotropy is so small that it can only be detected by ESR in our study. In conjunction with the quasi-two-dimensionality, our study establishes that Ba 3 MnSb 2 O 9 is a nearly ideal triangular lattice antiferromagnet with the quasiclassical spin S = 5/2, which suggests that it has the potential for an experimental study of Z- or Z 2 -vortex excitations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Barrierless nucleation in glassy precursors drives zeolite formation

Zeolites are crystalline, microporous silicates widely used in catalysis and separations, yet the molecular mechanisms of their formation remain unresolved. Experiments indicate that hydrothermal synthesis of silica zeolites from clear solution proceeds through amorphous nanoaggregates that gradually develop zeolite order in an apparently continuous amorphous to crystal transformation. Here, we combine molecular simulations with advanced algorithms that identify zeolite order and computer vision to elucidate the pathway from clear solution to zeolite nanocrystal. We show that at conditions of hydrothermal synthesis of silica zeolites, the transformation of precursor aggregate into zeolite is not limited by nucleation barriers but by the slow dynamics of reorganization in the glassy precursor matrix. The negligible nucleation barriers result in spinodal-like crystallization that leads to a gradual formation of a mosaic of small crystallites that explain the seemingly continuous character of zeolite crystallization and the catalytic activity of X-ray amorphous, protozeolites and embryonic zeolites. We find that zeolite-like porosity and short-range order emerge early within glassy precursors, well before crystallinity is detected in transmission electron microscopy (TEM) images or X-ray diffraction. The nanoaggregate’s temperature-size phase diagram reveals a convergence of the zeolite–amorphous equilibrium and maximum crystallization rate at ~3 nm diameter nanoparticle diameters and ~200 °C. This convergence signals the termination of the first-order amorphous-to-zeolite transition. Our results provide a unifying framework for understanding nucleation of silica zeolites from solution and suggest that barrierless nucleation may govern the formation of other nanoparticle systems, including minerals and oxides synthesized far below their bulk melting points.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Thermal properties of the metallic delafossite PdCo⁢O 2 : A combined experimental and first-principles study

Metallic delafossite materials (e.g., PdCo⁢O 2 , PtCo⁢O 2 ), have attracted much recent attention due to record-high oxide conductivities, the origins of which remain unclear. Relatively little attention has been paid to their related thermal properties, however. Here, we address this via wide temperature range experimental studies of the crystal structure, thermal expansion, and specific heat of single-crystal PdCo⁢O 2 , combined with density-functional theory (DFT) calculations of the electronic and phononic densities of states, and thus thermal properties. PdCo⁢O 2 is shown to retain the $R\bar{3}m$ space group from 12 to 1000 K, exhibiting a- and c-axis thermal expansion in good quantitative agreement with DFT-based lattice dynamics calculations. The Co-O bond lengths additionally elucidate the stability of the low-spin state of the nominally Co 3+ ions, which is a notable difference between the edge-shared Co-O octahedra in PdCo⁢O 2 and the corner-shared octahedra in Co-based perovskites. Measurements of specific heat from 1.9 to 400 K provide accurate values for the Debye temperature and Sommerfeld coefficient, the phononic part being describable via a combined Debye-Einstein approach (accounting for high-frequency oxygen-related optical phonons), with excess intermediate-temperature specific heat due to a prominent low-energy peak in the phonon density of states. Most significantly, all electronic and phononic contributions to the specific heat are shown to be remarkably closely reproduced by DFT-based calculations, establishing quantitative understanding of key thermal properties of the metallic delafossite PdCo⁢O 2 .

36 MATERIALS SCIENCE↗
DOE OSTI2025

Combining Theory and Experiment to Map the Atomic-Level Structure–Energy Pathways of Adsorbate-Mediated Phase Changes in a Cooperatively Flexible Metal–Organic Framework

An important subclass of metal–organic frameworks (MOFs) exhibits cooperative flexibility, wherein individual crystallites undergo global structural phase changes in response to external stimuli. Where cooperative flexibility results in reversible changes between crystalline states of distinct accessible porosity, these frameworks can exhibit rare yet desirable behaviors that cannot be explained by local dynamics alone. Yet, the chemical and structural origins of cooperative flexibility and how frameworks undergo these reversible phase changes at the atomic level remain poorly understood. Deliberate design for specific applications is therefore exceedingly difficult, and there is great impetus to develop a fundamental understanding of this phenomenon. Here, an effective and widely accessible computational approach is developed, which is designed to provide microscopic resolution via direct comparison to experimental data along the desorption-guided pathway. The strategy is applied to explain the desorption-induced phase change in an experimentally well-characterized framework, CdIF-13 (sod-Cd(benzimidazolate)2), where experiment alone was unable to resolve the atomistically detailed phase change landscape. Our findings reveal that the cooperative phase change pathways are adsorbate dependent with thermodynamics of intermediate structural states dictated by a nuanced interplay of ligand orientation, skeletal symmetry, and modes of surface adsorption. The results reveal that this isotropically flexible framework is “chaperoned” through a complex energy landscape by specific adsorbates, revealed by the reported computational approach with atomic-level insight and validated by experimentally determined structures. Thus, this work facilitates both understanding and future design of flexible materials for applications in gas storage, transport, delivery, and separation technologies.

03 NATURAL GAS↗
DOE OSTI2025

Structure and spectroscopy of graphite monofluoride

The structure of graphite monofluoride, (CF) n , has been debated since its discovery in 1934. In this work, we investigate a commercial graphite monofluoride by vibrational spectroscopy (infrared, Raman and the first inelastic neutron scattering spectra of this material). The spectroscopy shows that the material contains unreacted graphite and the partially fluorinated product dicarbon fluoride, (C 2 F) n , We evaluate the previously proposed $P\bar{6}m2$ and $P\bar{3}m1$ structures using computational methods and find F···F contacts render the $P\bar{6}m2$ structure dynamically unstable. We propose two alternative structures, $Cmc2_1$ $P6_3mc$, generated by displacement of one layer relative to another and find that $Cmc2_1$ is also dynamically unstable. The calculations are validated by comparison of calculated and observed INS spectra

Density functional theory↗
DOE OSTI2026

Quantum kinetic modeling of KEEN waves in a warm-dense regime

We report the first fully kinetic, quantum study of kinetic electrostatic electron nonlinear (KEEN) waves, showing that quantum diffraction systematically erodes the classical trapping mechanism, narrows harmonic locking to the fundamental, and hastens post-drive decay. Electrons are evolved with a second-order Strang-split 1D1V Wigner–Poisson solver that couples conservative semi-Lagrangian WENO advection to an analytic Fourier space update for the non-local Wigner term, while ions remain classical. We focus on collisionless dynamics in a weakly coupled regime, providing a controlled baseline before collisional extensions. Short, frequency-tuned ponderomotive pulses drive KEEN formation in a uniform Maxwellian plasma; as the dimensionless quantum parameter H rises from the classical limit to values relevant to warm-dense matter, doped semiconductors, and 2D electron systems, the drive threshold increases, higher harmonics are damped, trapped electron vortices diffuse, and the subplasma electrostatic energy relaxes to a lower stationary level, as confirmed by continuous wavelet analysis. These microscopic changes carry macroscopic weight. Ignition-scale capsules now compress matter to regimes where the electron de Broglie wavelength rivals the Debye length, making classical kinetic descriptions insufficient. By extending KEEN physics into this quantum domain, our results offer a potential diagnostic of non-equilibrium electron dynamics for next-generation inertial-confinement designs and high-energy-density platforms, indicating that predictive fusion modeling may benefit from the integration of kinetic fidelity with quantum effects.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Spin dynamics in natural multiferroic pyroxene NaFeSi 2 ⁢O 6

Spin dynamics in the natural mineral aegirine, NaFeSi 2⁢ O 6 , a member of the pyroxene family, was studied by elastic and inelastic neutron scattering. Magnetization and specific-heat measurements as well as single-crystal neutron diffraction maps, taken in the temperature range 2–20 K, confirm two successive magnetic transitions at 8.8 and 5.8 K, consistent with previous studies. The observed spin-wave excitations emerge from the incommensurate magnetic Bragg peaks corresponding to the propagation vector 𝑘 ICM = (0,0.77,0), and extend up to energies of about 1.5 meV. In the low-temperature helical phase, the spin dynamics of the Fe3+ ions is well described by a simple linear spin-wave model. The observed excitations can be modeled using a spin Hamiltonian that includes three primary exchange interactions—intrachain coupling 𝐽 = 0.142⁢(2) ⁢meV, and interchain couplings 𝐽 1 = 0.083⁢(1) ⁢meV and 𝐽 2 = 0.186⁢(1) meV—and an easy-plane anisotropy 𝐷 = 0.020⁢(6)⁢ meV. Furthermore, our results show that no single exchange interaction dominates the spin dynamics. The similar strengths of the intrachain and interchain couplings point to the fact that the magnetic interactions in aegirine are three dimensional rather than confined along one direction. As a result, the system cannot be considered quasi one dimensional, as previously suggested, and calls for further investigations.

Magnetic coupling↗
DOE OSTI2021

Multiphonon diffuse scattering in solids from first principles: Application to layered crystals and two-dimensional materials

Time-resolved diffuse scattering experiments have gained increasing attention due to their potential to reveal nonequilibrium dynamics of crystal lattice vibrations with full momentum resolution. Although progress has been made in interpreting experimental data on the basis of one-phonon scattering, understanding the role of individual phonons can be sometimes hindered by multiphonon excitations. In Ref. [M. Zacharias, H. Seiler, F. Caruso, D. Zahn, F. Giustino, P. C. Kelires, and R. Ernstorfer, Phys. Rev. Lett. 127, 207401 (2021)], we have introduced a rigorous approach for the calculation of the all-phonon inelastic scattering intensity of solids from first-principles. In the present work, we describe our implementation in detail and show that multiphonon interactions are captured efficiently by exploiting translational and time-reversal symmetries of the crystal. We demonstrate its predictive power by calculating the scattering patterns of monolayer molybdenum disulfide (MoS 2 ), bulk MoS 2 , and black phosphorus (bP), and we obtain excellent agreement with our measurements of thermal electron diffuse scattering. Remarkably, our results show that multiphonon excitations dominate in bP across multiple Brillouin zones, while in MoS 2 they play a less pronounced role. We expand our analysis for each system and examine the effect of individual atomic and interatomic vibrational motion on the diffuse scattering signals. We further demonstrate the high-throughput capability of our approach by reporting all-phonon scattering maps of two-dimensional MoSe 2 , WSe 2 , WS 2 , graphene, and CdI 2 , rationalizing in each case the effect of multiphonon processes. As a side point, we show that the special displacement method reproduces the thermally distorted configuration that generates precisely the all-phonon diffuse pattern. In conclusion, the present methodology opens the way for systematic calculations of the scattering intensity in crystals and the accurate interpretation of static and time-resolved inelastic scattering experiments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Calibration and characterization of the line-VISAR diagnostic at the HED-HIBEF instrument at the European XFEL

In dynamic-compression experiments, the line-imaging Velocity Interferometer System for Any Reflector (VISAR) is a well-established diagnostic used to probe the velocity history, including wave profiles derived from dynamically compressed interfaces and wavefronts, depending on material optical properties. Knowledge of the velocity history allows for the determination of the pressure achieved during compression. Such a VISAR analysis is often based on Fourier transform techniques and assumes that the recorded interferograms are free from image distortions. In this paper, we describe the VISAR diagnostic installed at the HED-HIBEF instrument located at the European XFEL along with its calibration and characterization. It comprises a two-color (532, 1064 nm), three-arm (with three velocity sensitivities) line imaging system. We provide a procedure to correct VISAR images for geometric distortions and evaluate the performance of the system using Fourier analysis. We finally discuss the spatial and temporal calibrations of the diagnostic. As an example, we compare the pressure extracted from the VISAR analysis of shock-compressed polyimide and silicon.

47 OTHER INSTRUMENTATION↗