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DOE OSTI2025

ATOMIC AND MICROSTRUCTURAL ORIGINS OF STORED ENERGY RELEASE IN NEUTRON-IRRADIATED SILICON CARBIDE

Here, we employ a combination of advanced synchrotron-based scattering characterization techniques to understand and unravel the atomic origins of the colossal stored energy release in neutron irradiated silicon carbide. The quantification of the neutron irradiation-induced defects, and their impact on the structureproperty relationship is important for the design and safe operation of advanced fission and fusion reactors. Our experimental results show that the atomic structure in the as irradiated samples is significantly perturbed due to a large fraction of vacancy and interstitial type defects that lead to complex microstructures and additional components in the x-ray diffraction and pair distribution function results. We directly correlate the stored energy release to the recovery of the sub-lattices, with pair distribution function analysis highlighting that the carbon interstitial and vacancy-type defects contribute to stored energy more than those of silicon. We find these results to be striking and believe our discoveries to be timely and noteworthy given the technological importance of silicon carbide to the nuclear fission and fusion communities.

Sprouster, D.J.↗

DOE OSTI2024

Evidence of short chains in liquid sulfur

High energy x-ray pair distribution function measurements show the average coordination number of the first shell in liquid sulfur is 1.86 ± 0.04 across the λ-transition, not precisely 2.0 as widely accepted. This indicates that upon melting, liquid sulfur does not comprise solely of S 8 rings but also possesses a significant number of short chains. Intensities of the pre-peak and first diffraction peak of the x-ray structure factor and third peak height of the pair distribution function all show deviations at the λ-transition temperature T λ , associated with the break-up of S 8 rings and the start of oligomer polymerization. A significant number of non-bonded or loosely bonded “interstitial atoms,” with an average coordination number of 0.20 ± 0.005, are also observed in the so-called “forbidden zone” between the first and second shells upon melting. The number of interstitial atoms is found to decrease to a minimum at the λ-transition, but the majority persist into the high temperature polymerized liquid. Furthermore, the existence of short chains and nearby interstitial atoms represent the two main factors required to initiate the S 8 -ring to chain transition, as proposed by recent molecular dynamics simulations.

Chemical bonding↗

DOE OSTI2025

Structure and Synthesizability of Iron–Sulfur Metal–Organic Frameworks

Sulfur-based metal–organic frameworks (MOFs) and coordination polymers (CPs) are an emerging class of hybrid materials that have received growing attention due to their magnetic, conductive, and catalytic properties with potential applications in electrocatalysis and energy storage. In this work, we report a high-throughput virtual screening protocol to predict the synthesizability of candidate metal–sulfur MOFs/CPs by computing the thermodynamically stable structures resulting from a particular combination of metal cluster, linker, cation, and synthetic conditions. Free energies are computed by using all-atom classical mechanical thermodynamic integration. Low-free-energy structures are refined using ab initio density functional theory, and pair distribution functions and powder X-ray diffraction patterns are calculated to complement and guide experimental structure determination. We validate the computational approach by retrospective predictions of the stable structure produced by experimental syntheses, and a subsequent screen predicts Fe 4 S 4 -BDT–TPP as a new thermodynamically stable one-dimensional (1D) CP comprising a redox-active Fe 4 S 4 cluster, a 1,4-benzenedithiolate (BDT) linker, and a tetraphenylphosphonium (TPP) countercation. Furthermore, this material is experimentally synthesized, and the 1D chain structure of the crystal is confirmed using microcrystal electron diffraction. The computational screening pipeline is generically transferable to neutral and ionic MOFs/CPs comprising arbitrary metal clusters, linkers, cations, and synthetic conditions, and we make it freely available as an open source tool to guide and accelerate the discovery and engineering of novel porous materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1990

Electron-positron heating and the eclipsing millisecond pulsar PSR 1957 + 20

The companion in the eclipsing millisecond PSR 1957 + 20 appears to be strongly heated by the pulsar and may also be rapidly losing mass due to that heating. A new mechanism is presented by which the heating may be accomplished: diffusion of mildly relativistic electron-positron pairs from the pulsar's relativistic wind through a thermal wind issuing from the companion. Wave-particle scattering regulates the depth at which the pairs deposit their energy; requirements of self-consistency place bounds on the wave spectrum and pair distribution function. If the pairs carry over about 10 percent of the pulsar spin-down luminosity, and the companion's heavy element abundance is subsolar, the heating rate can be adequate to drive a wind with sufficient momentum flux to explain the eclipse geometry. Annihilation photons then heat the companion beneath its photosphere and supply a significant part of the power for the optical luminosity. This model also suggests that the eclipse duration decreases sharply above a critical photon frequency.

Krolik, Julian H.↗

DOE OSTI2025

Investigating Quantum Materials with Half-Polarized Diffraction and magnetic PDF analysis at the HB-2A Neutron Powder Diffractometer

Local magnetic ordering and anisotropy is often central to the emergent behavior and subsequent functional properties in quantum materials and beyond. Neutron powder diffraction provides a straightforward yet extremely powerful technique for quantitative measurements of microscopic magnetic properties. The HB-2A powder diffractometer located at the High Flux Isotope Reactor in ORNL is traditionally utilized for long-range magnetic structure determination. Recently these capabilities have been extended to include methods aimed at accessing local magnetism: Half- polarized neutron powder diffraction (pNPD) and magnetic pair distribution function (mPDF) analysis. These two distinct techniques are possible on HB-2A due to the versatility of the instrument’s reciprocal space coverage, resolution and novel ultra-low temperature multi-sample changers that operate down to dilution refrigerator temperatures. This provides unique capabilities not found on any powder diffraction instrument and is particularly well suited to investigations of magnetic quantum materials. The development and implementation of these techniques will be discussed with a series of science case examples ranging from geometric frustrated magnets to magnetic metal-organic frameworks. Data reduction and analysis tools will be presented that enable the extraction of the local site susceptibility tensor and local spin-spin correlations in real space. Finally, potential combinations of these techniques in the form of half-polarized magnetic pair distribution function (pmPDF) analysis will be considered. Looking forward, HB-2A is undergoing a detector upgrade that will be in the user program by 2026. This will offer an order of magnitude increase in count rates to further aid the development of these often low signal measurements and provide new scientific capabilities.

Neutron Scattering↗

DOE OSTI2026

S 8 ring content in liquid sulfur determined from x-ray diffraction

The S 8 ring content in liquid sulfur has been determined from the 4.47 Å peak in the x-ray pair distribution function over the temperature range −55 °C –330 °C. This peak represents the characteristic 3rd and 4th nearest atom-atom distances across an S 8 -ring. Three procedures were used to calculate the S 8 -ring fraction; scaling to crystalline β-S, a linear combination fit and a direct integration method. All methods gave similar values, indicating that approximately one third of the S 8 -rings break up upon melting into a distribution of short chains with an average length of 5 ± 2 atoms. Our results contradict established models of low temperature sulfur that indicate below the λ-transition the liquid comprises almost entirely of S8-rings. In addition, we find the S 8 -ring fraction increases to 76 ± 10% at −30 °C in the supercooled liquid, and decreases to 23% ± 3% at 330 °C in the high temperature melt. First principle molecular dynamics calculations confirm the onset of dynamic ring distortion via broad bond angle distributions, associated with the interstitial region between the first and second peaks in the pair distribution function. Our results are consistent with the presence of a propensity of short chains in the low temperature liquid, that are required for the bond switching mechanism responsible for the polymerization process to occur at the λ-transition temperature, T λ .

lambda transition↗

DOE OSTI2024

Defect-Limited Mobility and Defect Thermochemistry in Mixed A-Cation Tin Perovskites: (CH3NH3)1-xCsxSnBr3

Hybrid organic-inorganic semiconductors crystallizing in the perovskite structure present a significant opportunity for realizing defect-tolerant semiconductors. In this work, we examine the solid solution, (CH3NH3)1-xCsxSnBr3, and identify the thermochemistry dictating the intrinsic carrier concentrations and how local structural distortions influences this electronic behavior. This family of compounds exhibits the expected systematic trend in decreasing optical gap with the cesium to methylammonium A-site mixing ratio, x, in the visible region. However, the carrier mobility, as determined from time-resolved microwave conductivity measurements, trends opposite to that expected from first-principles calculations combined with Boltzmann scattering theory calculations of the carrier mobility. We propose that this is a result of increasing carrier scattering with x in (CH3NH3)1-xCsxSnBr3 due to a significant increase in the carrier density with x. By examining the dependence of the carrier density as a function of x, we infer the compositional-dependence of the average enthalpy and nonconfigurational entropy per defect. While diffraction reveals a cubic aristotypic perovskite structure as a function of x at room temperature, the pair distribution functions obtained from synchrotron X-ray total scattering from these materials are better described by symmetry-adapted displacement modes of the Pm3m crystal structure, which we attribute to a large degree of anharmonic dynamics of the atom positions. This analysis shows that CH3NH3+-rich compositions retain mostly linear Sn-Br-Sn bonding environments through the displacements, while Cs+-rich compositions lead to more significantly bent Sn-Br-Sn environments. We propose that these bent bonding arrangements in Cs-rich compositions yield a higher propensity for defect formation. This also provides a rationale for carrier trapping that gives rise to anomalous microwave transients. Together, these results provide insight into the structure-dynamics-properties relationships in this highly anharmonic system with high amplitude atomic motions and low defect formation energies.

defect thermochemistry↗

DOE OSTI2025

Nucleation and growth of polar clusters with in-phase tilts into a long-range ferroelectric matrix in a sodium niobate based complex relaxor

In this study, we have investigated the temperature dependence of atomic ordering at multiple length scales in a lead-free sodium niobate-based relaxor, i.e., 0.75 NaNbO 3 -0.25 Ba 0.9⁢ Ca 0.1⁢ TiO 3 (NN-25BCT) via synchrotron x-ray diffraction, Raman spectroscopy, and pair distribution function analysis. High-resolution synchrotron x-ray powder diffraction (SXRD) measurements reveal a ferroelectric phase transition in the relaxor ferroelectric NN-25BCT below the Vogel-Fulcher freezing temperature (𝑇 VF ≈ 270 K). In addition, SXRD analysis demonstrates the competition between in-phase octahedral tilting and ferroelectric order at the long-range scale using mode crystallography. On the other hand, Raman spectroscopic analysis provides evidence of polar ordering for 𝑇 > 𝑇 VF (with tetragonal symmetry) persisting up to the Burns temperature (𝑇 B ). Furthermore, pair distribution function (PDF) analysis reveals the presence of a polar antiferrodistortive tetragonal phase with 𝑃⁢4⁢𝑏𝑚 space group at short ranges throughout the studied temperatures (i.e., 110 K ≤ 𝑇 ≤500 K), irrespective of nonpolar long-range ordering above 𝑇 VF . Therefore, our measurements provide direct evidence for the presence of polar ordering at short ranges and their gradual transformation into long-range polar ordering using an integrated multiscale structural analysis. In conclusion, as a result of a transition from relaxor to a ferroelectric phase in the vicinity of room temperature, NN-25BCT can be exploited for applications in pyroelectric detectors, electrocaloric devices, and multilayered ceramic capacitors.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Bridging Atomic Solvation Environment with Electrochemical Properties for the Bis(trifluoromethylsulfonyl)imide-Based Divalent Cation Electrolytes for the Next-Generation Energy Storage Systems

A deep molecular-level understanding of the multivalent electrolyte and its correlation with the electrochemical properties is crucial for designing optimized electrolytes for next-generation rechargeable batteries. Comprehensive knowledge of the atomic level of the solvation structure and its connection with electrochemical stability and ion transport properties is especially critical. However, the interaction of these three components coupled with clear atomistic insights is lacking in the literature. Here, our current contribution evaluates representative electrolytes with the bis(trifluoromethanesulfonyl)imide (TFSI) anions for multivalent cations of Mg, Ca, and Zn, at different ionic conditions with and without a cosolvated environment in ether-based solvent. Two critical problems are investigated: first, resolving the solvation structures in the electrolyte solutions as a function of concentrations through pair distribution function analysis and the corresponding electrochemical transport properties; second, unmasking the quantitative correlation of the atomistic environment with both electrochemical kinetics and cation dependence. We discovered that the magnesium- and calcium-based electrolytes display versatile coordination lengths but poor average anodic stability due to ion pairing with TFSI - . On the contrary, the zinc-based electrolytes show the shortest solvent coordination lengths, shielding the Zn cation from rigid solvent interactions and resulting in the highest anodic stabilities. Calcium-based electrolytes exhibit the longest and most concentration-independent coordination lengths. This work provides valuable insights into the molecular structural and electrochemical features of diverse multivalent electrolyte systems with cations in various solvation environments, emphasizing the importance of the solvation structure and construction in designing high-performance electrolytes.

cation coordination↗

NASA NTRS1989

Theory of droplet. Part 1: Renormalized laws of droplet vaporization in non-dilute sprays

The vaporization of a droplet, interacting with its neighbors in a non-dilute spray environment is examined as well as a vaporization scaling law established on the basis of a recently developed theory of renormalized droplet. The interacting droplet consists of a centrally located droplet and its vapor bubble which is surrounded by a cloud of droplets. The distribution of the droplets and the size of the cloud are characterized by a pair-distribution function. The vaporization of a droplet is retarded by the collective thermal quenching, the vapor concentration accumulated in the outer sphere, and by the limited percolative passages for mass, momentum and energy fluxes. The retardation is scaled by the local collective interaction parameters (group combustion number of renormalized droplet, droplet spacing, renormalization number and local ambient conditions). The numerical results of a selected case study reveal that the vaporization correction factor falls from unity monotonically as the group combustion number increases, and saturation is likely to occur when the group combustion number reaches 35 to 40 with interdroplet spacing of 7.5 diameters and an environment temperature of 500 K. The scaling law suggests that dense sprays can be classified into: (1) a diffusively dense cloud characterized by uniform thermal quenching in the cloud; (2) a stratified dense cloud characterized by a radial stratification in temperature by the differential thermal quenching of the cloud; or (3) a sharply dense cloud marked by fine structure in the quasi-droplet cloud and the corresponding variation in the correction factor due to the variation in the topological structure of the cloud characterized by a pair-distribution function of quasi-droplets.

Chiu, H. H.↗

NASA NTRS2003

Application of Powder Diffraction Methods to the Analysis of Short- and Long-Range Atomic Order in Nanocrystalline Diamond and SiC: The Concept of the Apparent Lattice Parameter (alp)

Two methods of the analysis of powder diffraction patterns of diamond and SiC nanocrystals are presented: (a) examination of changes of the lattice parameters with diffraction vector Q ('apparent lattice parameter', alp) which refers to Bragg scattering, and (b), examination of changes of inter-atomic distances based on the analysis of the atomic Pair Distribution Function, PDF. Application of these methods was studied based on the theoretical diffraction patterns computed for models of nanocrystals having (i) a perfect crystal lattice, and (ii), a core-shell structure, i.e. constituting a two-phase system. The models are defined by the lattice parameter of the grain core, thickness of the surface shell, and the magnitude and distribution of the strain field in the shell. X-ray and neutron experimental diffraction data of nanocrystalline SiC and diamond powders of the grain diameter from 4 nm up to micrometers were used. The effects of the internal pressure and strain at the grain surface on the structure are discussed based on the experimentally determined dependence of the alp values on the Q-vector, and changes of the interatomic distances with the grain size determined experimentally by the atomic Pair Distribution Function (PDF) analysis. The experimental results lend a strong support to the concept of a two-phase, core and the surface shell structure of nanocrystalline diamond and SiC.

Palosz, B.↗

DOE OSTI2025

Fast calculation of diffraction patterns from an ensemble of aligned molecules

We report an algorithm to calculate electron diffraction patterns for molecules with anisotropic angular distribution, which is significantly faster than existing methods. The algorithm uses a transform to convert the molecular orientation distribution, which is a function of three Euler angles, to the atom-pair distribution functions which depend on the polar and azimuthal angles. The diffraction signal can then be calculated from the atom-pair distributions. We demonstrate the computation method numerically by calculating electron diffraction patterns for a symmetric top molecule (trifluoroiodomethane) and an asymmetric top molecule (formaldehyde) and show that it reduces the calculation time by approximately two orders of magnitude compared to the standard brute-force method. Here, the method can also be applied to the calculation of x-ray diffraction patterns.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2024

Enhancing Low-Temperature Syngas Production via Surface Tailoring of Supported Intermetallic Nanocatalysts

An active and coke-resistant silica-encapsulated intermetallic Ni 3 Zn nanoparticle catalyst was developed for low-temperature (450 °C) dry reforming of methane (DRM). The catalyst exhibited a remarkable 4-fold increase in activity (4.5 s –1 ) with over 99% CO selectivity and 3 orders of magnitude less carbonaceous species and demonstrated remarkable stability (70 h) compared to that of a monometallic Ni catalyst. Here, the key is the combined effect of surface ensemble structure and electronic interaction modulation through the surface composition tailoring achieved by off-stoichiometric Ni and Zn loading in controlling surface chemistry for achieving different activities and H 2 /CO ratios. Characterized by ion spectroscopy, X-ray photoelectron spectroscopy, and the neutron pair distribution function, it was revealed that paired Ni δ – –Zn δ+ active sites are crucial for DRM. Transient infrared spectroscopy and isotopic analysis uncovered the synergistic effect of Ni δ – –Zn δ+ sites in activating C–H bonds and dissociating CO 2 to prevent coke formation under low-temperature conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1974

Critical point parameters of helium

Calculations of the critical point parameters of the helium isotopes using integral equation closures for the pair distribution function are reported for two pair potentials.

Bruch, L. W.↗

DOE OSTI2025

La 2 ⁢O 3 ⁢Mn 2 ⁢Se 2 : A correlated insulating layered d-wave altermagnet

Altermagnets represent a new class of magnetic phases without net magnetization, invariant under a combination of rotation and time reversal. Unlike conventional collinear antiferromagnets (AFM), altermagnets could lead to new correlated states and important material properties deriving from their nonrelativistic spin-split band structure. Indeed, they serve as the magnetic analogue of unconventional superconductors and can yield spin-polarized electrical currents in the absence of external magnetic fields, making them promising candidates for next-generation spintronics. Here, we report altermagnetism in the correlated insulator, magnetically ordered tetragonal oxychalcogenide, L⁢a 2 ⁢O 3⁢ M⁢n 2 ⁢S⁢e 2 . Symmetry analysis reveals a 𝑑 𝑥 2 −𝑦 2 -wave-like spin-momentum locking arising from the M⁢n 2 ⁢O Lieb lattice, supported by density functional theory (DFT) calculations. Magnetic measurements confirm the AFM transition below ∼166K while neutron pair distribution function analysis reveals a 2D short-range magnetic order that persists above the Néel temperature. Single crystals are grown and characterized using x-ray diffraction, optical and electron microscopy, and micro-Raman spectroscopy to confirm the crystal structure, stoichiometry, and uniformity. Furthermore, our findings establish L⁢a 2⁢ O 3 ⁢M⁢n 2⁢ S⁢e 2 as a model altermagnetic system realized on a Lieb lattice.

36 MATERIALS SCIENCE↗

DOE OSTI2024

X-ray and molecular dynamics study of the temperature-dependent structure of molten NaF-Zr⁢F 4

The local atomic structure of NaF-Zr⁢F 4 (53–47 mol%) molten system and its evolution with temperature are examined with x-ray scattering measurements which are then used to validate the quality of ab initio and neural network-based molecular dynamics (NNMD) calculations in the temperature range 515–700°⁢C. The machine-learning enhanced NNMD calculations offer improved efficiency while maintaining accuracy at higher distances compared to ab initio calculations. Looking at the evolution of the pair distribution function with increasing temperature, a fundamental change in the liquid structure within the selected temperature range, accompanied by a slight decrease in overall correlation is revealed. NNMD calculations indicate the coexistence of three different fluorozirconate complexes: [Zr⁢F 6 ] 2– , [Zr⁢F 7 ] 3– , and [Zr⁢F 8 ] 4– , with a shift in the dominant coordination state from the 7-coordinated Zr cation toward a 6-coordinated cation with increasing temperature. The study also highlights the metastability of different local coordination structures, with frequent interconversions between the 6- and 7-coordinate states. Analysis of the Zr-F-Zr angular distribution function reveals the presence of both “edge-sharing” and “corner-sharing” fluorozirconate complexes with specific bond angles and distances in accord with previous studies, while the next-nearest-neighbor cation-cation correlations demonstrate a clear preference for unlike cations as nearest-neighbor pairs, emphasizing nonrandom arrangement. Finally, these findings contribute to a comprehensive understanding of the complex local structure of the molten salt, providing insights into temperature-dependent preferences and correlations within the molten system.

36 MATERIALS SCIENCE↗

DOE OSTI2024

A bicarbonate-rich liquid condensed phase in non-saturated solutions in the absence of divalent cations

Bicarbonate (HCO 3 - ) and sodium (Na + )-containing solutions contain droplets of a separate, bicarbonate-rich liquid condensed phase (LCP) that have higher concentrations of HCO 3 - relative to the bulk solution in which they reside. The existence and composition of the LCP droplets has been investigated by nanoparticle tracking analysis, nuclear magnetic resonance spectroscopy, refractive index measurements and X-ray pair distribution function analysis. The bicarbonate-rich LCP species is a previously unaccounted-for, ionic phenomenon which occurs even in solutions with solely monovalent cations. Its existence requires re-evaluation of models used to describe and model aqueous solution physicochemistry, especially those used to describe and model carbonate mineral formation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Short-range magnetic order and planar anisotropy in the topological ferrimagnet Mn 3 ⁢Si 2 ⁢Te 6

Mn 3 ⁢Si 2 ⁢Te 6 is a ferrimagnetic topological nodal-line semiconductor that exhibits unconventional colossal magnetoresistance behavior, with short-range spin fluctuations being potentially intimately linked to the emergent properties. Here we determine the short-range magnetic order and anisotropy through total neutron scattering and polarized neutron powder diffraction measurements on polycrystalline Mn 3 ⁢Si 2⁢ Te 6 . Strong in-plane anisotropy is quantified on the Mn ions through extraction of the local site susceptibility tensor. Here, the real-space local spin structure is determined through the application of magnetic pair distribution function analysis covering a wide temperature range. Short-range order over a locally frustrated trimer of three nearest neighbors is found to exist well above the long-range ferrimagnetic transition.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗