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At least 523 records · Page 29
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Pressure-induced phase transition of calcite and aragonite: A first principles study

The thermodynamic phase stabilities of calcite and aragonite have been investigated from lattice vibrational analyses based on first-principles calculations. Different pressure dependences in phonon feature were found between the two polymorphs, suggesting different physical origins of the pressure-induced phase transitions. In the most stable phase in calcite (calcite I), an imaginary phonon mode consisting of rotation of CO{sub 3} ions with slight displacement of Ca ions appears at the F point in the Brillouin zone above 0.8 GPa. Such a soft mode means that external pressure induces the lattice-dynamical instability of calcite I leading to the phase transition to calcite II. On the other hand, the origin of the phase transition in aragonite is not due to such a lattice-dynamical instability. The estimated thermodynamical properties indicate that a first-order phase transition occurs between aragonite and post-aragonite at 34.7 GPa, coinciding with the reported experimental value at room temperature (35 GPa).

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS2012

Two Years of Simultaneous K(sub a)-Band Measurements: Goldstone, CA; White Sands, NM; and Guam, USA

In order to statistically characterize the effect of the Earth's atmosphere on Ka-Band links, site test interferometers (STIs) have been deployed at three of NASA s operational sites to directly measure each site's tropospheric phase stability and rain attenuation. These STIs are composed of two antennas on a short baseline (less than 1km) that observe the same unmodulated beacon signal broadcast from a geostationary satellite (e.g., Anik F2). The STIs are used to measure the differential phase between the two received signals as well as the individual signal attenuation at each terminal. There are currently three NASA sites utilizing STIs; the Goldstone Deep Space Communications Complex near Barstow, California; the White Sands Complex in Las Cruces, New Mexico; and the Guam Remote Ground Terminal on the island of Guam. The first two sites are both located in desert regions that have highly similar climates in terms of their seasonal temperatures, average humidity, and annual rain fall (the primary factors in determining phase stability). In contrast, Guam is in a tropical region with drastically higher annual rainfall and humidity. Five station years of data have been collected in Goldstone, three in White Sands, and two in Guam, yielding two years of simultaneous data collection across all three sites. During this period of simultaneous data collection, the root-mean-square (RMS) of the time delay fluctuations stayed under 2.40 picoseconds for 90% of the time in Goldstone, under 2.07 picoseconds for 90% of the time in White Sands, and under 10.13 picoseconds for 90% of the time in Guam. For the 99th percentile, the statistics were 6.32 ps, 6.03 ps, and 24.85 ps, respectively. These values, as well as various other site quality characteristics, will be used to determine the suitability of these sites for NASA s future communication services at Ka-Band.

Acosta, Roberto J.↗
DOE OSTI2021

High-efficiency perovskite photovoltaic modules achieved via cesium doping

Perovskite solar modules have been attracting increasing attention due to their market potential, yet publications concerned with theintrinsic scale-up potential of different perovskite compositions remain relatively scarce. On the other hand, while great success is being made towards improving the power conversion efficiency (PCE) of perovskite solar cells (PSCs) by cesium cation (Cs + ) doping of the perovskite, more attention is being paid to the perovskite phase stabilization effect of Cs + doping, and less to other properties that are critical to understand and futher improve the PSC's. In this work, moderately-Cs-doped MAPbI 3 was employed as a model perovskite material in order to exclude the phase stabilization effect. Our systematic study revealed the influence of Cs + in organic-inorganic hybrid perovskites on the crystal structure, crystallization process, trap state density, band structure and charge (i.e., ions or photo-carriers) transport. Markedly, it has been observed that Cs + doping can greatly increase the carrier diffusion length in the perovskite films, thus improving the potential to scale-up PSC's.The PCE of small area devices (0.09 cm 2 ) was increased to 21.72% from 19.73%, with decreased hysteresis behavior and increased operational stability (T85 = 1000 h) after Cs + doped, where T85 refers to the retention of 85% of the initial PCE. Moreover, a PCE of 21.08% was obtained for a Cs + -containing perovskite module with an active area > 30 cm 2 , which demonstrates a better "reproducibility" than the reference sample (MAPbI3-based perovskite modules, PCE = 18.26%).

14 SOLAR ENERGY↗
DOE OSTI2013

Phase transition and possible metallization in CeVO{sub 4} under pressure

Phase stability of CeVO{sub 4} under pressure has been investigated using synchrotron based angle dispersive x-ray diffraction (ADXRD), electrical resistance and first principles calculations. The results indicate that the ambient zircon structure of the compound transforms to a low symmetry monoclinic monazite phase beyond 3.8 GPa with nearly 8.6% volume discontinuity. Beyond 11 GPa, the pattern could be fitted to a similar monazite structure which is about 12.7% denser and has a much larger monoclinic beta angle. On pressure release the first monoclinic phase is recovered. The electrical resistance data show a large drop in resistance with pressure indicating substantial narrowing down of the band gap. Electronic structure calculations support these observations and suggest possible pressure induced metallization in this material. - Pressure induced structural phase transition in CeVO{sub 4} as observed by x- ray diffraction (pressure vs. volume) and possible metallization in CeVO{sub 4} through electrical resistance and first principles electronic structure calculations. - Highlights: • Structural and electrical behavior of CeVO{sub 4} under pressure studied using x-ray diffraction and electrical resistance measurements and first principles calculations. • Two successive structural transitions confirmed by experiment and theory: zircon–monazite I–monazite II. • Band gap collapse and possible metallization is indicated by electrical resistance measurements and electronic structure calculations under pressure. • Novel observation of lower bulk modulus in the high pressure phase (both by experiment and calculations) explained through structural analysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

The Effect of η Phase Precipitates on the Creep Behavior of Alloy 263 and Variants

Phase stability is an important design parameter for Ni-based superalloys to be used in future advanced ultra-supercritical (AUSC) power plants as exposure times in this type of environment are considerable. In this investigation, microstructures based on candidate alloy 263 were obtained with varying amounts of η precipitates using isothermal exposure at 800°C for times ranging from 1,000 h to 10,000 h. The effect of η phase stability on the creep properties was determined using creep specimens isothermally aged at 800°C for 8 h, 3,000 h, 5,000 h and 10,000 h prior to creep screening. The creep life was found to exponentially decrease with increasing density of η phase while the elongation to failure was found to increase. Furthermore, the minimum creep rate was related to the density of η phase; a relationship that did not depend on the alloy formulation. Modification to the Ti and Al concentrations slowed down the γ' to η transformation while doubling the γ' fraction after standard heat treatment. By modifying the Ti and Al content, and thereby improving γ' stability over η, the creep lives of specimens isothermally aged for up to 5,000 h were greater than that of the nominal alloy in its standard aged condition.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Understanding the microstructural stability in a y’-strengthened Ni-Fe-Cr-Al-Ti alloy

Ni-Fe-Cr-Al-Ti alloys, with Ni levels near 50 wt.%, have the potential to develop a microstructure consisting of a face-centered cubic ? matrix with the homogeneous precipitation of fine ordered ?’ precipitates similar to traditional Ni-based superalloys with significantly greater Ni content. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), atom probe tomography (APT), and CALPHAD -based thermodynamic modeling were employed to understand the phase stabilities and microstructural evolution in an age-hardenable Ni-27Fe-18Cr-1Co-1.6Al-3.75Ti-1.2Mo-0.03C (wt%) alloy. The primary heat-treatment of solution annealing at 1121°C for 4h and age-hardening treatment at 760 °C for 16h resulted in a microstructure consisting of fine ?’ precipitates in an austenitic matrix along with grain boundary carbides, consistent with thermodynamic calculations. Long-term aging at 900 °C for 250h resulted in the coarsening of ?’ along with a change in the morphology of the precipitates from spherical to a more cuboidal shape. In addition, ? phase formation was observed concomitant with the partial dissolution of the ?’ phase. The ability of computational thermodynamic models to predict microstructural characteristics is discussed.

Gwalani, Bharat↗
DOE OSTI2015

Phase engineering of monolayer transition-metal dichalcogenide through coupled electron doping and lattice deformation

First-principles calculations were performed to investigate the phase stability and transition within four monolayer transition-metal dichalcogenide (TMD) systems, i.e., MX{sub 2} (M = Mo or W and X = S or Se) under coupled electron doping and lattice deformation. With the lattice distortion and electron doping density treated as state variables, the energy surfaces of different phases were computed, and the diagrams of energetically preferred phases were constructed. These diagrams assess the competition between different phases and predict conditions of phase transitions for the TMDs considered. The interplay between lattice deformation and electron doping was identified as originating from the deformation induced band shifting and band bending. Based on our findings, a potential design strategy combining an efficient electrolytic gating and a lattice straining to achieve controllable phase engineering in TMD monolayers was demonstrated.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

Additive Manufacturing of Hierarchical Multi-Phase High-Entropy Alloys for Nuclear Component

In recent years, high entropy alloys (HEAs), composed of four or more metallic elements mixed in equal or near equal atomic percent, have attracted significant attention due to their excellent mechanical properties and good corrosion resistance. They show significant promise as candidates for high temperature fission and fusion structural applications. However, the conventional synthesis methods are unlikely to present an industrially suitable route for the production and use of HEAs. Recognizing rapidly evolving additive manufacturing (AM) techniques, the goal of this proposal is to optimize the AM process to fabricate HEAs with predesigned chemical compositions and phase morphologies for nuclear components. For this project, two HEAs FeCrNiMn and FeCrNiMnAl have been successfully synthesized. Correlated mechanical response has been systematically characterized under a variety of laser processing and ion irradiations. Both high entropy alloys are found to present comparable swelling and extraordinary irradiation tolerance (limited voids and stabilized phase structure under high irradiation dose). In addition, the microstructure and radiation-induced hardening can be tailored by laser processing under additive manufacturing. And we have assembled at LANL a unique database of HEAs containing a total of 674 compositions with Phase Stability information. Based on this, the machine learning and Artificial Intelligence capability now are established to predict the microstructure of casted HEAs by given chemical compositions. This unique integration will lead to an optimal AM recipe for fabricating radiation tolerant HEAs. The development of both modeling models and experimental capability will also benefit other programs at LANL.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Thermal equation of state of ice-VII revisited by single-crystal X-ray diffraction

Abstract Ice-VII is a high-pressure polymorph of H2O ice and an important mineral widely present in many planetary environments, such as in the interiors of large icy planetary bodies, within some cold subducted slabs, and in diamonds of deep origin as mineral inclusions. However, its stability at high pressures and high temperatures and thermoelastic properties are still under debate. In this study, we synthesized ice-VII single crystals in externally heated diamond-anvil cells and conducted single-crystal X-ray diffraction experiments up to 78 GPa and 1000 K to revisit the high-pressure and high-temperature phase stability and thermoelastic properties of ice-VII. No obvious unit-cell volume discontinuity or strain anomaly of the high-pressure ice was observed up to the highest achieved pressures and temperatures. The volume-pressure-temperature data were fitted to a high-temperature Birch-Murnaghan equation of state formalism, yielding bulk modulus KT0 = 21.0(4) GPa, its first pressure derivative KT0′ = 4.45(6), dK/dT = –0.009(4) GPa/K, and thermal expansion relation αT = 15(5) × 10–5 + 15(8) × 10–8 × (T – 300) K–1. The determined phase stability and thermoelastic properties of ice-VII can be used to model the inner structure of icy cosmic bodies. Combined with the thermoelastic properties of diamonds, we can reconstruct the isomeke P-T paths of ice-VII inclusions in diamond from depth, offering clues on the water-rich regions in Earth’s deep mantle and the formation environments of those diamonds.

Geochemistry & Geophysics↗
DOE OSTI2017

Computational investigation of half-Heusler compounds for spintronics applications

We present first-principles density functional calculations of the electronic structure, magnetism, and structural stability of 378 XYZ half-Heusler compounds (with X= Cr, Mn, Fe, Co, Ni, Ru, Rh; Y=Ti, V, Cr, Mn, Fe, Ni; Z= Al, Ga, In, Si, Ge, Sn, P, As, Sb). We find that a “Slater-Pauling gap” in the density of states (i.e., a gap or pseudogap after nine states in the three atom primitive cell) in at least one spin channel is a common feature in half-Heusler compounds. We find that the presence of such a gap at the Fermi energy in one or both spin channels contributes significantly to the stability of a half-Heusler compound. We calculate the formation energy of each compound and systematically investigate its stability against all other phases in the open quantum materials database (OQMD). Here, we represent the thermodynamic phase stability of each compound as its distance from the convex hull of stable phases in the respective chemical space and show that the hull distance of a compound is a good measure of the likelihood of its experimental synthesis. We find low formation energies and mostly correspondingly low hull distances for compounds with X= Co, Rh, or N, Y= Ti or V, and Z= P, As, Sb, or Si. We identify 26 18-electron semiconductors, 45 half-metals, and 34 near half-metals with negative formation energy that follow the Slater-Pauling rule of three electrons per atom. Our calculations predict several new, as-yet unknown, thermodynamically stable phases, which merit further experimental exploration—RuVAs, CoVGe, FeVAs in the half-Heusler structure, and NiScAs, RuVP, RhTiP in the orthorhombic MgSrSi-type structure. Further, two interesting zero-moment half-metals, CrMnAs and MnCrAs, are calculated to have negative formation energy. In addition, our calculations predict a number of hitherto unreported semiconducting (e.g., CoVSn and RhVGe), half-metallic (e.g., RhVSb), and near half-metallic (e.g., CoFeSb and CoVP) half-Heusler compounds to lie close to the respective convex hull of stable phases, and thus may be experimentally realized under suitable synthesis conditions, resulting in potential candidates for various semiconducting and spintronics applications.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Coherent two-dimensional Fourier transform spectroscopy using a 25 Tesla resistive magnet

We performed nonlinear optical two-dimensional Fourier transform spectroscopy measurements using an optical resistive high-field magnet on GaAs quantum wells. Magnetic fields up to 25 T can be achieved using the split helix resistive magnet. Two-dimensional spectroscopy measurements based on the coherent four-wave mixing signal require phase stability. Therefore, these measurements are difficult to perform in environments prone to mechanical vibrations. Large resistive magnets use extensive quantities of cooling water, which causes mechanical vibrations, making two-dimensional Fourier transform spectroscopy very challenging. Here, we report on the strategies we used to overcome these challenges and maintain the required phase-stability throughout the measurement. A self-contained portable platform was used to set up the experiments within the time frame provided by a user facility. Furthermore, this platform was floated above the optical table in order to isolate it from vibrations originating from the resistive magnet. Finally, we present two-dimensional Fourier transform spectra obtained from GaAs quantum wells at magnetic fields up to 25 T and demonstrate the utility of this technique in providing important details, which are obscured in one dimensional spectroscopy.

47 OTHER INSTRUMENTATION↗
DOE OSTI2026

Design, Processing, and Properties of WTaCrV-Hf Multi-principal Element Alloys

Refractory multi-principal element alloys are candidates for high-temperature structural components due, in part, to their high strength and high melting points. Single-phase materials are initially preferred for isotropic material properties as a function of time and temperature in service conditions. This work outlines a computational rank-ordering and experimental validation methodology for single-phase body-centered-cubic phase stability in WTaCrV-Hf alloys using order–disorder transition temperature. Eight compositions were fabricated by arc-melting and heat-treated at 1400 °C for 24 hrs. X-ray diffraction, energy-dispersive x-ray spectroscopy, and Vickers hardness testing showed alloys with order–disorder transition temperatures below 600 °C formed a single-phase body-centered-cubic structure during solidification and remained single-phase after heat-treatment. The sample possessing the lowest order–disorder transition temperature exhibited slip traces suggestive of room-temperature plastic deformation under Vickers indentation, with both heat-treated single-phase samples exhibiting hardnesses over 800 HV with little cracking compared to tungsten. These results establish order–disorder transition temperature as a viable predictive parameter for multi-principal element alloy phase stability. The methodology outlined in this work provides a framework for future design, fabrication, and characterization of high-temperature structural multi-principal element alloys.

CALPHAD↗
DOE OSTI2012

Synthesis and Characterization of Thiazolium-Based Room Temperature Ionic Liquids for Gas Separations

A series of novel thiazolium-bis(triflamide) based ionic liquids has been synthesized and characterized. Physicochemical properties of the ionic liquids such as thermal stability, phase transitions, and infrared spectra were analyzed and compared to the imidazolium-based congeners. Several unique classes of ancillary substitutions are examined with respect to impacts on overall structure, in addition to their carbon dioxide absorption properties in supported ionic-liquid membranes for gas separation.

Hillesheim, PC↗
DOE OSTI2015

Abnormal cubic-tetragonal phase transition of barium strontium titanate nanoparticles studied by in situ Raman spectroscopy and transmission electron microscopy heating experiments

Phase stability of the ferroelectric materials at high temperature is extremely important to their device performance. Ba{sub x}Sr{sub 1−x}TiO{sub 3} (BST) nanoparticles with different Sr contents (x = 1, 0.91, 0.65, 0.4, and 0) are prepared by a facile hydrothermal method. Using Raman spectroscopy and transmission electron microscopy (TEM) analyses under in situ heating conditions (up to 300 °C), the phase transitions of BST nanoparticles between 25 °C and 280 °C are comprehensively investigated. The original Curie temperature of BST nanoparticles decreases abruptly with the increase in Sr content, which is more obvious than in the bulk or film material. Besides, an abnormal phase transition from cubic to tetragonal structure is observed from BST nanoparticles and the transition temperature rises along with the increase in Sr content. Direct TEM evidences including a slight lattice distortion have been provided. Differently, BaTiO{sub 3} nanoparticles remained in the tetragonal phase during the above temperature ranges.

36 MATERIALS SCIENCE↗
NASA NTRS2008

L-Band Transmit/Receive Module for Phase-Stable Array Antennas

Interferometric synthetic aperture radar (InSAR) has been shown to provide very sensitive measurements of surface deformation and displacement on the order of 1 cm. Future systematic measurements of surface deformation will require this capability over very large areas (300 km) from space. To achieve these required accuracies, these spaceborne sensors must exhibit low temporal decorrelation and be temporally stable systems. An L-band (24-cmwavelength) InSAR instrument using an electronically steerable radar antenna is suited to meet these needs. In order to achieve the 1-cm displacement accuracy, the phased array antenna requires phase-stable transmit/receive (T/R) modules. The T/R module operates at L-band (1.24 GHz) and has less than 1- deg absolute phase stability and less than 0.1-dB absolute amplitude stability over temperature. The T/R module is also high power (30 W) and power efficient (60-percent overall efficiency). The design is currently implemented using discrete components and surface mount technology. The basic T/R module architecture is augmented with a calibration loop to compensate for temperature variations, component variations, and path loss variations as a function of beam settings. The calibration circuit consists of an amplitude and phase detector, and other control circuitry, to compare the measured gain and phase to a reference signal and uses this signal to control a precision analog phase shifter and analog attenuator. An architecture was developed to allow for the module to be bidirectional, to operate in both transmit and receive mode. The architecture also includes a power detector used to maintain a transmitter power output constant within 0.1 dB. The use of a simple, stable, low-cost, and high-accuracy gain and phase detector made by Analog Devices (AD8302), combined with a very-high efficiency T/R module, is novel. While a self-calibrating T/R module capability has been sought for years, a practical and cost-effective solution has never been demonstrated. By adding the calibration loop to an existing high-efficiency T/R module, there is a demonstrated order-of-magnitude improvement in the amplitude and phase stability.

Andricos, Constantine↗
DOE OSTI2020

Thermal conductivity of (Ge 2 Sb 2 Te 5 ) 1–x Cx phase change films

Germanium–antimony–telluride has emerged as a nonvolatile phase change memory material due to the large resistivity contrast between amorphous and crystalline states, rapid crystallization, and cyclic endurance. Improving thermal phase stability, however, has necessitated further alloying with optional addition of a quaternary species (e.g., C). In this work, the thermal transport implications of this additional species are investigated using frequency-domain thermoreflectance in combination with structural characterization derived from x-ray diffraction and Raman spectroscopy. Specifically, the room temperature thermal conductivity and heat capacity of (Ge 2 Sb 2 Te 5 ) 1–x C x are reported as a function of carbon concentration (x ≤ 0:12) and anneal temperature (T ≤ 350 °C) with results assessed in reference to the measured phase, structure, and electronic resistivity. Phase stability imparted by the carbon comes with comparatively low thermal penalty as materials exhibiting similar levels of crystallinity have comparable thermal conductivity despite the addition of carbon. The additional thermal stability provided by the carbon does, however, necessitate higher anneal temperatures to achieve similar levels of structural order.

42 ENGINEERING↗
DOE OSTI2019

Mn(II) oxidation catalyzed by nanohematite surfaces and manganite/hausmannite core-shell nanowire formation by self-catalytic reaction

The present study investigated the solid products of heterogeneous catalytic oxidation of aqueous Mn(II) by O2 in the presence of hematite nanoparticles (NPs) using transmission electron microscopy (TEM), scanning TEM (STEM), and electron energy-loss spectroscopy (EELS). The oxidation experiments were conducted at room temperature (22±2?) in solutions containing 10-3 M Mn(II) at pH 7.5 in the dark. During 48 hours of reaction, a single-phase manganite (a Mn oxyhydroxide) nanowire was formed by way of metastable groutite and feitknechtite nanowires, both of which are polymorphs of manganite. Between 48 and 168 hours, the manganite further altered to core-shell structured nanowires with hausmannite (a mixed valent Mn oxide) forming a very thin (2 nm) outer-shell on the manganite wire core. The formation of Mn-oxyhydroxide nanowires was catalyzed by the hematite NPs surface through electrochemical pathways. This is described via the electron transfer across a redox couple from adsorbed Mn(II) to another site with adsorbed O2 via the band structure of the semiconducting hematite. On the other hand, the Ostwald step rule was operative in the sequential crystallization from metastable groutite and feitknechtite to stable manganite, which could have resulted from the differences in the surface free energies, sizes, and morphologies of product polymorphs at the nanoscale. The final product (at least in the time range of our experiments) exhibited manganite/hausmannite core-shell structures. This product is most likely to be formed by the reactions catalyzed by the manganite nanowires themselves. Microscopic investigation of interfacial changes in structure and chemistry at the nanoscale is key, and it can be essential to understand the kinetic and thermodynamic phenomena related to the redox chemistry and phase stability of nanoparticles in complex, heterogeneous systems such as natural environments.

Inoue, Sayako↗
DOE OSTI2023

Computationally Accelerated Discovery and Experimental Demonstration of High-Performance Materials for Advanced Solar Thermochemical Hydrogen Production

This project achieved its overarching goal of accelerating the discovery and validation of solar thermochemical hydrogen (STCH) materials through a tightly integrated approach that combined high-throughput computational screening, advanced machine learning (ML), and experimental testing. Guided by the objectives outlined in the Statement of Project Objectives (SOPO), our work fulfilled all major milestones across four technical tasks and delivered scientific breakthroughs and practical tools that significantly exceeded the original scope of the project. We began by addressing the challenge of predicting material phase stability through machine learning. A novel Python module was developed to generate thousands of meaningful features from composition, structure, and electronic properties, enabling rapid and reproducible ML model development. Using these tools, we trained a model to predict temperature-dependent Gibbs energies (G(T)) for inorganic crystalline materials with near-chemical accuracy—roughly 40 meV/atom—marking the first such descriptor of its kind. We also introduced a new machine-learned tolerance factor, τ, that accurately predicted perovskite formability with over 90% success, outperforming traditional heuristic models, such as the Goldschmidt tolerance factor. These capabilities allowed for rapid and accurate predictions of phase stability across a vast oxide composition space, setting the stage for high-throughput thermodynamic screening. Building on this foundation, we conducted an extensive computational screening of candidate STCH oxide materials. Over 1.1 million perovskite compositions were evaluated using the τ descriptor, leading to the identification of more than 27,000 predicted stable structures. Using density functional theory (DFT), we refined over 68,000 multinary perovskite structures and computed oxygen vacancy formation energies for over 1,300 ternary and double perovskites. These calculations enabled us to isolate compounds with redox behavior consistent with STCH requirements and resulted in a public dataset now hosted on the Materials Project. Recognizing that thermodynamic screening alone is insufficient, we addressed kinetic limitations by developing a suite of tools to estimate transition state (TS) energies for key redox reactions. We implemented a novel bounding approach that provides lower and upper estimates of TS energies with dramatically reduced computational cost, requiring less than 10% of the CPU time of a full nudged elastic band (NEB) calculation while maintaining high accuracy. This enabled rapid evaluation of over 200 reaction pathways across 90 materials. To further accelerate screening, we developed a SISSO-based ML model to predict diffusion barriers with a 96.7% success rate in classifying fast vs. slow materials, supporting a robust, data-driven framework for assessing redox kinetics. Experimental validation was critical to confirming the predictive power of our models. We synthesized and tested a wide array of candidate materials, including Mn-doped hercynite and several Gd- and La-based perovskites. Notably, Sr 0.4 Gd 0.6 Mn 0.6 Al 0.4 O 3 (SGMA) and Gd 0.5 La 0.5 Co 0.5 Fe 0.5 O 3 (GLCF) emerged as leading STCH materials, exhibiting robust redox cycling and high hydrogen yields exceeding 150 µmol H 2 /g per cycle. These materials also retained over 50% of their hydrogen productivity under high-conversion conditions (H 2 O:H 2 = 1333:1), demonstrating strong thermodynamic favorability and promising performance under industrially relevant scenarios. Additional candidates, such as La 2 MnNiO 6 (L2MN), were found to produce even higher yields than ceria under standard STCH conditions. Our collaborators at Sandia National Laboratories confirmed these findings using high-temperature X-ray diffraction and thermogravimetric analysis, observing stable phase evolution and reversible redox activity. In several respects, the project went beyond the goals initially outlined in the SOPO. We published 17 peer-reviewed articles, including a large dataset of over 66,000 theoretical perovskites and a new structure prediction method (SPuDS-DFT) that accurately identifies ground-state structures at a fraction of the cost of traditional DFT. We demonstrated that our machine-learned G(T) model offers accuracy rivaling quasiharmonic calculations while being orders of magnitude faster. In partnership with the Materials Project, we made our datasets openly available, providing a powerful new resource for the broader materials science community. The combined computational and experimental advances of this project represent a significant advance in STCH materials discovery. By creating a robust, generalizable, and open workflow for thermodynamic and kinetic screening, and validating key findings through synthesis and reactor testing, we have provided a practical and scalable pathway for the rapid identification of new redox-active materials. The tools, data, and materials developed under this project are already supporting ongoing research and have laid the groundwork for the next generation of solar fuel technologies.

08 HYDROGEN↗