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DOE OSTI2024

Chemical randomness, lattice distortion and the wide distributions in the atomic level properties in high entropy alloys

High entropy alloys (HEAs) consist of multiple elements present in large proportions that are randomly distributed on a crystal lattice. On the one hand, the presence of multiple elements engenders wide ranges of atomic radii, electronegativities, electron valences and magnetic moments, whereas on the other, the presence of chemical randomness creates unique nearest neighbor environments among the lattice sites. As a result, the symmetry of the energy landscape is broken essentially at each lattice site thereby resulting in highly distorted energy landscapes. At the atomistic level, the lattice distortion has been widely observed in the form of varying bond lengths. At the electronic level, a range of charge transfers result in the charge density distortion. Collectively, the distorted landscapes cause large quantitative variations of the atomic level properties; in this review, we highlight the effect of lattice distortion on point defect energetics, stacking fault energies, and dislocation mobility. Besides the well- known large HEAs phase space, the enormity of the distorted energy landscape that scales with the atomic configurations is a new consideration; understanding this coupling between composition, lattice distortion and properties’ variations thus becomes an exciting but challenging area within the field of HEAs. Furthermore, this coupling is expected to open a new door for materials design, where the materials properties could be tuned via leveraging the lattice distortion, which is essentially absent in dilute/ordered alloys.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Towards additive manufacturing of magnetocaloric working materials

The feasibility of three-dimensional printing via the Directed Energy Deposition (DED) technique is demonstrated for the ferromagnetic AlFe 2 B 2 (aka 1-2-2) compound, which shows promise as a working material for room-temperature magnetocaloric devices. Like many intermetallic materials, the 1-2-2 compound is brittle at room temperature; not only is it difficult to synthesize from the melt, it is challenging to form it into useful geometries necessary for effective heat transfer in magnetocaloric devices. Using Laser Engineered Net Shaping (LENS TM ) synthesis from two powder precursors, AlB 2 and Fe, samples of simple (rod) and complex (honeycomb) architectures were successfully synthesized. Furthermore, the phase constitution and distribution, magnetic transition temperature, and saturation magnetization determined for the LENS TM -synthesized rod sample are all similar to those obtained for 1-2-2 materials made by conventional casting. Further, the measured magnetic entropy change, as determined from Maxwell's Relations applied to magnetic data, indicates that the magnetocaloric response of the annealed LENS TM -printed rod samples are comparable to those of the 1-2-2 compounds made by conventional techniques. These results confirm that complex magnetofunctional shapes, which are needed for efficient energy conversion in magnetocaloric devices, can be rapidly fabricated from the AlFe 2 B 2 compound.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Spinel high-entropy oxides (FeNiCrMnZnX) 3 O 4 (X = Al, mg) as anode materials for high-performance lithium-ion batteries

To address the high cost, cobalt dependency, and resource constraints typical of conventional high-entropy oxide (HEO) anodes, this study reports the successful synthesis of two Co-free, six-component spinel-type HEOs(FeNiCrMnZnAl) 3 O 4 (HEO-Al) and (FeNiCrMnZnMg) 3 O 4 (HEO-Mg), via a sol-gel method. The distinct effects of Al 3+ and Mg 2+ incorporation on the electrochemical performance and lithium storage kinetics were systematically investigated. XRD, Raman, and TEM characterizations confirm that both materials possess a pure spinel phase, uniform particle size, and homogeneous elemental distribution. Notably, electrochemical evaluations reveal that HEO-Al delivers a superior reversible capacity of 480.7 mAh g −1 after 100 cycles at 0.1 A g −1 , and maintains 354.5 mAh g −1 after 1000 long-term cycles at 1 A g −1 , significantly outperforming HEO-Mg. Kinetic analysis indicates that HEO-Al exhibits lower charge transfer resistance, a higher Li + diffusion coefficient, and a pseudocapacitive contribution of up to 82%. Furthermore, these findings demonstrate that Al substitution effectively optimizes the structural stability and lithium storage kinetics of Co-free HEOs, providing a viable strategy for designing low-cost, highly stable HEO anode systems.

Anode materials↗

DOE OSTI2021

Information transfer with a gravitating bath

Late-time dominance of entanglement islands plays a critical role in addressing the information paradox for black holes in AdS coupled to an asymptotic non-gravitational bath. A natural question is how this observation can be extended to gravitational systems. To gain insight into this question, we explore how this story is modified within the context of Karch-Randall braneworlds when we allow the asymptotic bath to couple to dynamical gravity. We find that because of the inability to separate degrees of freedom by spatial location when defining the radiation region, the entanglement entropy of radiation emitted into the bath is a time-independent constant, consistent with recent work on black hole information in asymptotically flat space. If we instead consider an entanglement entropy between two sectors of a specific division of the Hilbert space, we then find non-trivial time-dependence, with the Page time a monotonically decreasing function of the brane angle---provided both branes are below a particular angle. However, the properties of the entropy depend discontinuously on this angle, which is the first example of such discontinuous behavior for an AdS brane in AdS space.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2024

Impact of Synthetic Parameters on Structure and Electrochemistry of High-Entropy Layered Oxide LiNi 0.2 Co 0.2 Mn 0.2 Al 0.2 Fe 0.2 O 2

Here, this study explored a high-entropy layered oxide (HELO), LiNi 0.2 Co 0.2 Mn 0.2 Al 0.2 Fe 0.2 O 2 , prepared by coprecipitation followed by heat treatment. Coprecipitation yielded a kinetically favored product, and the subsequent heat treatment under various temperatures and times allowed tuning the material toward more thermodynamically favored structures. Refinement of X-ray powder diffraction (XRD) revealed that after 450 °C treatment, ~12% of the Ni 2+ in the structure was located within the lithium cation layer. After heat treatment at 600, 700, and 800 °C, there was a continued decrease of Ni 2+ in the lithium cation layer to 9.3, 6.3, and 3.7%, respectively. Longer heat treatment times at 800 °C decreased the level to 2.5%. Electrochemical behavior was evaluated by cyclic voltammetry, galvanostatic cycling, rate capability testing, and electrochemical impedance spectroscopy, where increased loaded voltage, functional capacity, rate capability, and decreased impedance were observed for samples treated at higher temperatures with lower cation mixing. X-ray absorption near edge spectroscopy (XANES) data indicated that the redox activity of Ni and Co was dominant in the electrochemistry, while the participation of Mn or Fe was minimal. The level of Ni oxidation state change between charge and discharge related to the heat treatment temperature where the samples with high cation mixing showed lower capacity consistent with some Ni 3+ in the transition metal layer inaccessible for electron transfer. Longer heat treatment times at 800 °C did not continue to provide a benefit in electrochemical function even with some additional reduction in cation mixing.

25 ENERGY STORAGE↗

DOE OSTI2025

Joining Study for Formed Plate Heat Exchangers (CRADA Final Report)

Plate heat exchangers (PHEs) have been used in numerous industrial applications, such as HVAC systems, power generation, transportation and manufacturing. The performance of plate heat exchangers is frequently undermined by corrosion, fouling, and scaling. These phenomena not only diminish heat transfer efficiency but also lead to increased operational costs, maintenance demands, and reduced equipment lifespan. In this project, the team addressed the widespread challenges of corrosion, fouling, and scaling, and explored alternative material solutions. While commonly used materials like stainless steel and titanium offer notable benefits, they can still experience corrosion under certain operating conditions. The advancement of new materials and surface engineering technologies, such as advanced coating, ceramics, composites materials, and high entropy alloys are promising for can help solve these issues, enable longer lifetime and high performance of plate heat exchangers.

99 GENERAL AND MISCELLANEOUS↗

DOE OSTI2025

Joining Study for Formed Plate Heat Exchangers (Final Report)

36 MATERIALS SCIENCE↗

DOE OSTI2023

Automated reaction kinetics and network exploration (Arkane): A statistical mechanics, thermodynamics, transition state theory, and master equation software

The open-source statistical mechanics software described here, Arkane–Automated Reaction Kinetics and Network Exploration–facilitates computations of thermodynamic properties of chemical species, high-pressure limit reaction rate coefficients, and pressure-dependent rate coefficient over multi-well molecular potential energy surfaces (PES) including the effects of collisional energy transfer on phenomenological kinetics. Arkane can use estimates to fill in information for molecules or reactions where quantum chemistry information is missing. The software solves the internal energy master equation for complex unimolecular reaction systems. Inputs to the software include converged electronic structure computations performed by the user using a variety of supported software packages (Gaussian, Molpro, Orca, TeraChem, Q-Chem, Psi4). The software outputs high-pressure limit rate coefficients and pressure-dependent phenomenological rate coefficients, as well as computed thermodynamic properties (enthalpy, entropy, and constant pressure heat capacity) with added energy corrections. Some of the key features of Arkane include treatment of 1D, 2D or ND hindered internal rotation modes, treatment of free internal rotation modes, quantum tunneling effect consideration, transition state theory (TST) and Rice-Ramsperger-Kassel-Marcus (RRKM) rate coefficient computations, master equation solution with four implemented methods, inverse-Laplace transform of high-pressure limit rate coefficients into the energy domain, energy corrections based on bond-additivity or isodesmic reactions, automated and efficient PES exploration, and PES sensitivity analysis. The present work describes the design of Arkane, how it should be used, and refers to the theory that it employs. Arkane is distributed via the RMG-Py software suite (https://github.com/ReactionMechanismGenerator/RMG-Py).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Solvent Reorganization and Surface–Species Interactions Control Transfer Hydrogenation Rates in Sn-Beta Zeolites

Reorganization of confined alcohol networks reshapes adsorption and activation thermodynamics in Lewis acid zeolites, yet the roles of adsorbate sterics and non-H-bonding cosolvents remain unclear. Here, we investigate transfer hydrogenation of methyl- (mCH) and tert-butylcyclohexanone (tbCH) with 2-butanol over hydrophobic Sn-Beta. First-order rates per defect-open Sn site are 2–5× higher for mCH than tbCH, but converge in the zero-order regime (333–393 K), indicating that solvent reorganization entropically drives adsorption, while bond activation is insensitive to ketone structure. Reactions in toluene or acetonitrile (with 1 M 2-butanol) show that intraporous solvent organization governs transition-state stabilization: on hydrophobic Sn-Beta, apparent enthalpies and entropies rise with decreasing solvent polarity, whereas hydrophilic zeolites display nearly constant barriers across solvents. Liquid-phase IR spectroscopy corroborates these trends, showing that hydrophilic pores enforce 2-butanol-like solvation environments even in toluene. Together, these results reveal how zeolite pores regulate the intraporous solvent structure, whose reorganization upon adsorption reshapes the thermodynamic landscape of Lewis acid catalysis

Adsorption↗

DOE OSTI2022

Entanglement entropy and non-local duality: Quantum channels and quantum algebras

Here, we investigate the transformation of entanglement entropy under dualities, using the Kramers–Wannier duality present in the transverse field Ising model as our example. Entanglement entropy between local spin degrees of freedom is not generically preserved by the duality; instead, entangled states may be mapped to states with no local entanglement. To understand the fate of this entanglement, we consider two quantitative descriptions of degrees of freedom and their transformation under duality. The first involves Kraus operators implementing the partial trace as a quantum channel, while the second utilizes the algebraic approach to quantum mechanics, where degrees of freedom are encoded in subalgebras. Using both approaches, we show that entanglement of local degrees of freedom is not lost; instead it is transferred to non-local degrees of freedom by the duality transformation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Noble Gas Transport in the MSRE

This study explores the relationship between the physicochemical parameter known as Henry’s gas constant and gas transport across a two-layer film interface. The investigation utilized the Gibbs free energy, incorporating surface and volume terms to elucidate trends in enthalpy and entropy. Notably, our findings align with experimental data and offer predictive insights into the Henry’s gas constants for helium and krypton, which hold significance for future experiments and theoretical developments. Furthermore, this study enhances the Gibbs free energy theory pertaining to the liquid–gas interface. It underscores the substantial contribution of noble gases in this region to volumetric energy as temperature increases. Additionally, we employed Monte Carlo simulations to analyze the effective thermal neutron multiplication factor, denoted as k eff . Our analysis reveals a linear correlation between graphite density and uniform density as a function of temperature. For the 1D Molten Salt Reactor Experiment (MSRE) system, we employed the Mole code to conduct heat and mass transfer calculations. These computations enable us to ascertain the distribution of fuel temperature based on coefficients and thermal properties. We also studied delayed neutron precursors during fuel cycling, taking into account the drift of cycling fuel through Mole–Griffin coupling. Our model represents k eff and β eff across various volume flow rates and salinity compositions. Finally, this study leveraged xenon-135 for continuous on-line monitoring of fuel salts to investigate the impact of steady-state xenon-135 on the MSRE and to better understand its distribution. These efforts build upon previous research related to removal processes.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2023

Enthalpy-uphill exciton dissociation in organic/2D heterostructures promotes free carrier generation

Despite the large binding energy of charge transfer (CT) excitons in type-II organic/2D heterostructures, it has been demonstrated that free carriers can be generated from CT excitons with a long lifetime. Using a model fluorinated zine phthalocyanine (F 8 ZnPc)/monolayer-WS 2 interface, we find that CT excitons can dissociate spontaneously into free carriers despite it being an enthalpy-uphill process. Specifically, it is observed that CT excitons can gain an energy of 250 meV in 50 ps and dissociate into free carriers without any applied electric field. This observation is surprising because excited electrons typically lose energy to the environment and relax to lower energy states. Here, we hypothesize that this abnormal enthalpy-uphill CT exciton dissociation process is driven by entropy gain. Kinetically, the entropic driving force can also reduce the rate for the reverse process – the conversion of free electron–hole pairs back to CT excitons. Hence, this mechanism can potentially explain the very long carrier lifetime observed in organic/2D heterostructures.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Experimental and computational kinetics study of the liquid-phase hydrogenation of C=C and C=O bonds

Solvent effects on adsorption equilibrium and reaction kinetics are evaluated for hydrogenation reactions catalyzed by Pd/alumina in a series of different solvents. Three reactants – cyclohexene, benzene and benzaldehyde – and three solvents – n-heptane (HEP), methylcyclohexane (MCHA), decalin (DL) – have been investigated. Kinetic analysis of hydrogenation of cyclohexene reveals that hydrogen adsorbs on different sites from those where cyclohexene and the solvents adsorb; however, the presence of hydrogen on these separate sites affects the heats of adsorption of the hydrocarbons. When the solvent is a weakly interacting linear alkane (HEP), the rate determining step of the reaction is the first hydrogenation of adsorbed cyclohexene. Furthermore, this conclusion is supported by DFT calculations that show a higher enthalpy barrier for the first hydrogenation than for the second, while statistical thermodynamics analysis validates the physical significance of the entropy of adsorption parameters derived from the kinetic fitting of experimental data. By contrast, with solvents such as MCHA and DL, which interact more strongly with the metal surface and compete for active sites with the reactant and the surface intermediate, the rate limiting step seems to shift to the second hydrogenation step.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Multi-task graph neural networks for simultaneous prediction of global and atomic properties in ferromagnetic systems *

Abstract We introduce a multi-tasking graph convolutional neural network, HydraGNN, to simultaneously predict both global and atomic physical properties and demonstrate with ferromagnetic materials. We train HydraGNN on an open-source ab initio density functional theory (DFT) dataset for iron-platinum with a fixed body centered tetragonal lattice structure and fixed volume to simultaneously predict the mixing enthalpy (a global feature of the system), the atomic charge transfer, and the atomic magnetic moment across configurations that span the entire compositional range. By taking advantage of underlying physical correlations between material properties, multi-task learning (MTL) with HydraGNN provides effective training even with modest amounts of data. Moreover, this is achieved with just one architecture instead of three, as required by single-task learning (STL). The first convolutional layers of the HydraGNN architecture are shared by all learning tasks and extract features common to all material properties. The following layers discriminate the features of the different properties, the results of which are fed to the separate heads of the final layer to produce predictions. Numerical results show that HydraGNN effectively captures the relation between the configurational entropy and the material properties over the entire compositional range. Overall, the accuracy of simultaneous MTL predictions is comparable to the accuracy of the STL predictions. In addition, the computational cost of training HydraGNN for MTL is much lower than the original DFT calculations and also lower than training separate STL models for each property.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

MS25: Materials Science-Focused Benchmark Data Set for Machine Learning Interatomic Potentials

Here, we present MS25, a benchmark data set for evaluating machine learning interatomic potentials (MLIPs) across diverse materials-relevant systems including MgO surfaces, liquid water, zeolites, a catalytic Pt surface reaction, high-entropy alloys (HEAs), and disordered Zr-oxides. Five MLIP architectures (MACE, NequIP, Allegro, MTP, and Torch-ANI) are trained and tested, focusing not only on traditional metrics (energies, forces, and stresses) but also explicitly validating derived physical observables such as lattice constants, volumes, and reaction barriers. We find that most models reach comparable accuracy on standard error metrics across the simple systems, although equivariant MLIPs offer 1.5–2× improvements over nonequivariant MLIPs in energy and force error for structurally complex or compositionally disordered environments such as HEAs and Zr–O systems. Our analysis highlights that low errors in energy and force predictions do not guarantee reliable observables, emphasizing the necessity of explicit validation. We demonstrate limitations in cross-framework transferability, as models trained on one zeolite framework (CHA) fail to reliably generalize to predictions of structurally distinct frameworks (e.g., MFI). Size-extensive tests show some dependence on system size for MgO, resulting from forced periodicity. The HEA and Zr–O data sets are identified as challenging tests for future benchmarks and MLIP model architecture developments as they show significant differentiation in error between MLIP architectures and are still relatively difficult at 1000 training images. Moving forward, we recommend that benchmarking efforts shift their focus from marginal accuracy improvements in energy and force errors toward identifying and understanding model failure modes, rigorously assessing transferability, and evaluating how their errors affect observable predictions. For researchers looking to choose an MLIP architecture, we suggest selecting equivariant MLIP architectures if the complexity of the system is a challenge. For simple materials problems, auxiliary features such as integration with molecular dynamics engines, trade-offs between computational data set generation cost vs MLIP inference speed, and framework integration may play a more important decision factor than small differences in error metrics that are unlikely to matter for production-level research.

chemical structure↗

DOE OSTI2025

Intrinsic activation energies for ring contraction of allylic cations in zeolites

Cyclic carbocations are important intermediates in zeolite-catalyzed chemistries such as methanol-to-hydrocarbons conversion, naphthenes ring opening, or coke formation. While information about their thermodynamic stability exists, little is known about the kinetics of formation and transformation of cyclic carbocations in zeolites. To fill this knowledge gap, ring contraction of the 1,3,5,5-tetramethylcyclohexenyl cation (C 10 H 17 + ), a representative of 6-membered ring allylic cations, was investigated by in situ UV–vis and IR spectroscopy. Protonic forms of zeolites served as catalysts, at temperatures from 80 °C to 135 °C. Significant oligomerization and hydride transfer in BEA and FAU hampered kinetics analysis, whereas ring contraction dominated in the channels of MOR. The reactant cation, characterized by an electronic absorption at 314 nm and an allylic stretch at 1549 cm −1 , contracted to both a 1,3-alkyl-substituted cyclopentenyl cation (287 nm and 1506 cm −1 ) and a 1,2,3-alkyl-substituted cyclopentenyl cation (297 nm and 1489 cm −1 ). Collection of time-resolved IR spectra and fitting of the intensities with various kinetic models revealed a third transformation, which is expected from thermodynamics: the 1,3-alkyl-substituted cyclopentenyl cation isomerizes to the 1,2,3-alkyl-substituted cyclopentenyl cation. Series of IR spectra recorded at different temperatures delivered intrinsic activation enthalpies (entropies) in MOR of 67 ± 2 kJ mol −1 (−130 ± 6 J mol −1 K −1 ) and 90 ± 3 kJ mol −1 (−70 ± 8 J mol −1 K −1 ) for the contraction to 1,3- and 1,2,3-substituted species, and of 88 ± 5 kJ mol −1 (−84 ± 12 J mol −1 K −1 ) for the isomerization. The findings characterize one path – via contraction of larger rings – to different cyclopentenyl species in zeolites; and the associated, moderate activation energies suggest such transformations contribute to many complex hydrocarbon reaction networks.

Acid catalysis↗

DOE OSTI2023

Quantitative Simulations of Siloxane Adsorption in Metal–Organic Frameworks

We present a transferable force field (FF) for simulating the bulk properties of linear and cyclic siloxanes and the adsorption of these species in metal–organic frameworks (MOFs). Unlike previous FFs for siloxanes, our FF accurately reproduces the vapor–liquid equilibria of each species in the bulk phase. The quality of our FF combined with the Universal Force Field using standard Lorentz–Berthelot combining rules for MOF atoms was assessed in a wide range of MOFs without open metal sites, showing good agreement with dispersion-corrected density functional theory calculations. Predictions with this FF show good agreement with the limited experimental data for siloxane adsorption in MOFs that is available. As an example of using the FF to predict adsorption properties in MOFs, we present simulations examining entropy effects in binary linear and cyclic siloxane mixture coadsorption in the large-pore MOF with structure code FOTNIN.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Laser-direct-drive fusion target design with a high- Z gradient-density pusher shell

Laser-direct-drive fusion target designs with solid deuterium-tritium (DT) fuel, a high-Z gradient-density pusher shell (GDPS), and a Au-coated foam layer have been investigated through both 1D and 2D radiation-hydrodynamic simulations. Compared with conventional low-Z ablators and DT-push-on-DT targets, these GDPS targets possess certain advantages of being instability-resistant implosions that can be high adiabat (α ≥ 8) and low hot-spot and pusher-shell convergence (CR hs ≈ 22 and CR PS ≈ 17), and have a low implosion velocity (v imp < 3 × 10 7 cm/s). Using symmetric drive with laser energies of 1.9 to 2.5 MJ, 1D LILAC simulations of these GDPS implosions can result in neutron yields corresponding to >~50–MJ energy, even with reduced laser absorption due to the cross-beam energy transfer (CBET) effect. Two-dimensional DRACO simulations show that these GDPS targets can still ignite and deliver neutron yields from 4 to ~10 MJ even if CBET is present, while traditional DT-push-on-DT targets normally fail due to the CBET-induced reduction of ablation pressure. If CBET is mitigated, these GDPS targets are expected to produce neutron yields of >20 MJ at a driven laser energy of ~2 MJ. Here are the key factors behind the robust ignition and moderate energy gain of such GDPS implosions are as follows: (1) The high initial density of the high-Z pusher shell can be placed at a very high adiabat while the DT fuel is maintained at a relatively low-entropy state; therefore, such implosions can still provide enough compression ρR >1 g/cm 2 for sufficient confinement; (2) the high-Z layer significantly reduces heat-conduction loss from the hot spot since thermal conductivity scales as ~1/Z; and (3) possible radiation trapping may offer an additional advantage for reducing energy loss from such high-Z targets.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗