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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 1,153 records · Page 64
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Predicting Thermochemical Equilibria with Interacting Defects: Sr 1 − x Ce x Mn O 3 − δ Alloys for Water Splitting

Solar thermochemical hydrogen is one of the few potential routes towards direct fuel production from renewable energy sources, but the thermodynamic boundary conditions for efficient and economic energy conversion are challenging. Success or failure of a given oxide working material depends on the subtle balance between enthalpy and entropy contributions in the redox processes. Developing a mechanistic understanding of the behavior of materials on the basis of atomistic models and first-principles calculations is an important part of advancing the technology. One challenge is to quantitatively predict thermochemical equilibria at high concentrations when the redox-active defects start to interact with each other, thereby impeding the formation of additional defects. This problem is of more general importance to applications that rely on high levels of off-stoichiometry or doping, including, for example, batteries, thermoelectrics, and ceramic fuel cells. To account for such repulsive defect interactions, we introduce a statistical mechanics approach, defining an expression for the free energy of defect interaction based on limited sampling of defect configurations in density functional theory supercell calculations. The parameterization of this energy contribution as a function of defect concentration and temperature allows on-the-fly simulation of thermochemical equilibria. The approach consistently incorporates finite temperature effects by including the leading contributions to the temperature-dependent free energy for the case at hand, i.e., the ideal gas and configurational enthalpies and entropies. We demonstrate the capability and utility of the approach by simulating the water splitting redox processes for Sr 1 − x Ce x Mn O 3 − δ alloys. Published by the American Physical Society 2024

08 HYDROGEN↗
DOE OSTI2026

Mechanistic Insights for Plasma-Catalytic CO 2 Reduction over TiO 2 in a Dielectric Barrier Discharge Reactor

Reaction kinetics experiments coupled with phenomenological kinetic modeling and parameter estimation are used to elicit insights into the mechanism and active sites for the plasma-catalytic dissociation of CO 2 on TiO 2 . Experimental and model insights showed that gas-phase reactions contribute at least two-thirds of the overall product formation at explored conditions; weak temperature dependence, strong sensitivity to specific energy input (SEI), apparent first order in CO 2 , and positive influence of cofed argon (Ar) and oxygen (O 2 ) for the gas-phase contributions all suggest that expected plasma reaction steps such as electron-impact and high-energy collisions are the dominant modes for CO 2 dissociation. The Arrhenius-like expression for gas contributions resulted in a preexponential of 4.40 × 10 –3 s –1 , an E SEI,g of 7.90 × 10 –4 mol/kJ, and an E a,g of 1.00 × 10 –3 J/mol. For surface contributions, the small apparent barrier of 16.3 kJ/mol, relatively weaker dependence on SEI, first-order dependence on CO 2 , and insensitivity to cofed Ar and O 2 all point to CO 2 dissociation on TiO 2 surface facets without vacancies and aided by plasma (leading to vibrationally excited CO 2 and/or a reactive surface with significant surface charge accumulation). The Arrhenius-like expression resulted in a preexponential of 7.81 × 10 –2 s –1 , an E SEI,s of 1.90 × 10 –3 mol/kJ, and an E a,s of 1.63 × 10 4 J/mol. The derived kinetic model further enabled a systematic evaluation of the effect of inputs (plasma power, flow rate, CO 2 inlet concentration, and temperature) to identify process trends and optimal operating conditions.

catalyst↗
DOE OSTI2020

Critical nuclei at hetero-phase interfaces

Two-step nucleation, in which a metastable intermediate phase acts as a precursor for nucleating a thermodynamically stable phase, has been widely observed in many materials systems and solid-state reactions. Among the advantages of two-step nucleation is that the stable phase may nucleate heterogeneously at the hetero-phase interface between the original and the precursory phases. Although heterogeneous nucleation (HN) theories for homo-phase grain boundaries and inert surfaces are well established, our understanding of HN at reactive hetero-phase interfaces remains incomplete. This deficiency stems from the discontinuity of the chemical potential driving force across the hetero-phase interface, which profoundly affects the fundamental properties of the nucleus in a way that is not properly accounted for in existing models. In this work, we incorporate these effects to extend the classical nucleation theory to HN at hetero-phase interfaces. Our extended model demonstrates that the nucleus shape along the minimum energy path is strongly size-dependent, and this additional degree of freedom can result in the reduction of the critical nucleus volume and associated activation energy barrier by orders of magnitude relative to conventional predictions. The simulation results are used to construct a sensitivity map in the parameter space of interfacial energy and bulk driving force ratios, which quantifies the difference in nucleation barriers predicted by different models.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Hamiltonian simulation in the low-energy subspace

Abstract We study the problem of simulating the dynamics of spin systems when the initial state is supported on a subspace of low energy of a Hamiltonian H . This is a central problem in physics with vast applications in many-body systems and beyond, where the interesting physics takes place in the low-energy sector. We analyze error bounds induced by product formulas that approximate the evolution operator and show that these bounds depend on an effective low-energy norm of H . We find improvements over the best previous complexities of product formulas that apply to the general case, and these improvements are more significant for long evolution times that scale with the system size and/or small approximation errors. To obtain these improvements, we prove exponentially decaying upper bounds on the leakage to high-energy subspaces due to the product formula. Our results provide a path to a systematic study of Hamiltonian simulation at low energies, which will be required to push quantum simulation closer to reality.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2024

Effect of Co on twin formation and magnetic properties of Sm(Fe,Ti,V) 12 alloys

Transferring the excellent intrinsic magnetic properties of SmFe 12 -based compounds to their extrinsic properties remains the main challenge in the development of high-performance SmFe12-based permanent magnets. Twin formation is one of the reasons for the inability to achieve high coercivity and remanence. Here we have shown that the addition of Co in Sm(Fe 1-x Co x ) 10–11 M 1–2 alloys, where M=Ti and V, leads to an increase in twin density. Microstructural characterizations revealed that the atomic arrangement in the twin boundary changes depending on the stabilizing element, which directly influences the local intrinsic magnetic properties. Theoretical investigations showed that the critical grain size at which twin formation can be hindered by grain size reduction decreases when the stabilizer changes from V to Ti. Furthermore, this study shows that the alloy composition influences not only the intrinsic magnetic properties but also the twin formation energy and its grain size dependence, crucial for the design of SmFe12-based permanent magnets.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Shuttling Majorana zero modes in disordered and noisy topological superconductors

The braiding of Majorana zero modes (MZMs) forms the fundamental building block for topological quantum computation. Braiding protocols which involve the physical exchange of MZMs are typically envisioned on a network of topological superconducting wires. An important component of these protocols is the transport of MZMs, which can be performed by using electric gates to locally tune sections of the wire between topologically trivial and nontrivial phases. In this work, we numerically simulate this transport by tuning a single section of a superconducting wire which contains either disorder (uncorrelated and correlated) or noise. We focus on the impact of these additional effects on the diabatic error, which describes unwanted transitions between the ground state and excited states. We show that the behavior of the average diabatic error is predominantly controlled by the statistics of the minimum bulk energy gap which is suppressed in the presence of disorder. The increase in diabatic error can be several orders of magnitude and is most deleterious when the disorder correlation length is a finite fraction of the transport distance and negligible when these lengths are far apart. In the presence of noise, the diabatic error is significantly enhanced due to optical transitions which depend on the minimum bulk energy gap as well as the frequency modes present in the noise. The results presented here serve to further characterize the diabatic error in disordered and noisy settings, which are important considerations in practical implementations of physical braiding schemes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Characterization of nuclear breakup as a function of hard-scattering kinematics using dijets measured by ATLAS in p+Pb collisions

This Letter analyzes the sensitivity of event geometry estimators to the initial-state kinematics of hard scattering in proton–lead collisions. This analysis uses dijets as a proxy for the parton–parton scattering configuration, correlating it with event geometry estimators, namely the energy deposited in the Zero-Degree Calorimeter and the transverse energy recorded in the Forward Calorimeter in the Pb-going direction. The analysis uses data recorded by the ATLAS detector at the Large Hadron Collider with a nucleon–nucleon center-of-mass energy of 8.16 TeV, corresponding to an integrated luminosity of 56 nb − 1 . The jets are measured within the pseudorapidity interval −2.8 < η < 4.5, where positive η values correspond to the direction of the proton beam. Results are presented as a function of the Bjorken-x of the parton originating from the proton, xp . Both event geometry estimators are found to be dependent on xp , with the energy deposited in the Zero-Degree Calorimeter about six times less sensitive to xp compared with the transverse energy deposited in the Forward Calorimeter.

Aad, G↗
DOE OSTI2024

Imaging the wakes of jets with energy-energy-energy correlators

As the partons in a high energy jet propagate through the droplet of quark-gluon plasma (QGP) produced in a heavy-ion collision they lose energy to, kick, and are kicked by the medium. The resulting modifications to the parton shower encode information about the microscopic nature of QGP. A direct consequence, however, is that the momentum and energy lost by the parton shower are gained by the medium and, since QGP is a strongly coupled liquid, this means that the jet excites a wake in the droplet of QGP. After freezeout, this wake becomes soft hadrons with net momentum in the jet direction meaning that what an experimentalist later reconstructs as a jet includes hadrons originating from both the modified parton shower and its wake. This has made it challenging to find experimental observables that provide an unambiguous view of the dynamical response of a droplet of QGP to a jet shooting through it. Recent years have seen significant substantial advances in the theoretical and experimental understanding of the substructure of jets, in particular, using correlation functions, $\langle$ ($\vec{n}$ 1 )•••$\mathcal{E}$($\vec{n}$ k ) $\rangle$, of the energy flux operator in proton-proton collisions and, recently, in heavy-ion collisions. So far, such studies have focused primarily on the two-point correlator, which allows for the identification of the angular scale of the underlying dynamics. Higher-point correlators hold the promise of mapping out the dynamics themselves. In this paper we perform the first study of the shape-dependent three-point energy-energy-energy correlator in heavy-ion collisions. Using the Hybrid Model to simulate the interactions of high energy jets with the QGP medium, we show that the three-point correlator presents us with a striking new opportunity. We find that hadrons originating from wakes are the dominant contribution to the three-point correlator in the kinematic regime in which the three points are well-separated in angle, forming a roughly equilateral triangle. This equilateral region of the correlator is far from the region populated by collinear vacuum emissions, making it a canvas on which jet wakes are laid out, where experimentalists can map their shapes. Our work provides a key step towards the systematic use of energy correlators to image and unravel the dynamical response of a droplet of QGP that has been probed by a passing jet, and motivates numerous experimental and theoretical studies.

Jets and Jet Substructure↗
DOE OSTI2022

Resolution of zigzag magnetic correlations in Na-deficient Na x IrO 3 without long-range ordering

The materials search for Kitaev quantum spin liquids led to the discovery of many honeycomb lattice materials. Much attention has been paid to materials without magnetic order down to the lowest temperatures. The newly synthesized Na-deficient Na x IrO 3 has been found to bear no sign of long-range magnetic order above 1 K from physical property measurements. In this paper, we report momentum-and energy-resolved excitation spectra in Na-deficient Na x IrO 3 measured using a resonant inelastic x-ray scattering spectrometer. Orbital excitation spectra show that the octahedral and trigonal crystal field splittings are larger in Na x IrO 3 than in Na 2 IrO 3 . On the other hand, the low-energy spectrum at low temperature shows a wave-vector dispersion and a spectral weight distribution that are similar to those of Na 2 IrO 3 , revealing that the two-dimensional zigzag magnetic correlations in Na x IrO 3 are similar to those in Na 2 IrO 3 in terms of the ordered magnetic moment direction and three dynamically fluctuating zigzag orders. The azimuth angle dependence of the low-energy spectrum corroborates these results. The two-dimensional zigzag magnetic correlations rapidly weaken until 50 K. At high temperatures, the spectral weight distribution of the low-energy excitation resembles that of the pure Kitaev model, indicating that the Kitaev interaction dominates the dynamic magnetic response at high temperature. Here we suggest that the larger crystal field and distortion and the weakened longer-range Heisenberg exchange interactions due to the Na deficiency in Na x IrO 3 contribute to bring Na x IrO 3 away from the zigzag long-range magnetic order phase.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Operating Strategies for Dispatchable PEM Electrolyzers that Enable Low-Cost Hydrogen Production

Hydrogen is a pathway to enabling decarbonization across multiple economic sectors that cannot be directly decarbonized with electricity including heat for industrial operations, medium- and heavy-duty transportation applications, long-duration energy storage, and as a feedstock for chemical synthesis. Producing hydrogen at low costs and carbon footprint is likely essential to economically decarbonize these otherwise "hard to decarbonize" sectors. Low-temperature polymer electrolyte membrane (PEM) electrolysis produces hydrogen from water and electricity and is a rapidly developing pathway towards making hydrogen at the scales required for decarbonization applications. The levelized cost of electrolytic hydrogen is dependent on the capital cost, efficiency, and durability of the electrolyzer system as well as the price of electricity supplied to the electrolyzer and the annual utilization of the electrolyzer (capacity factor). Electricity price and capacity factor depend on the source of energy that the system uses and impact other economic factors. Electricity price and capacity factor and the connections between other aspects of hydrogen production via PEM electrolyzers are the focus of this work. PEM electrolyzers have conventionally been operated at high capacity factors using electricity purchased from utilities with a constant price throughout the year. To achieve lower effective electricity prices, recent work has investigated opportunities for electrolyzers to purchase electricity in wholesale markets, where the cost of electricity varies hourly. This option can lead to lower electricity costs when the electrolyzer is a controllable load that ramps up and down rapidly and turns on and off frequently. This configuration and operating strategy capitalizes on times of low wholesale electricity prices and results in lower hydrogen levelized costs than constant operation due to reduced electricity costs even though the reduced capacity factor increases the cost of recovering the capital investment. Cycling on and off frequently also has implications for electrolyzer durability. An electrolyzer configuration where it is directly connected to renewable generation such as wind or solar, only running when the generator is producing energy, has similar implications on operating strategy, hydrogen levelized cost, capacity factor, and durability. This work provides insight into the relationships between dispatchable electrolyzer operating strategies and the cost of producing hydrogen from these systems, outlining strategies and opportunities to minimize production costs while minimizing operations that are likely to negatively impact system durability and efficiency. We find strategies that minimize electrolyzer cycling and the resulting durability impacts while increasing the hydrogen levelized cost only slightly above the minimum. We also find opportunities for batteries to minimize the number of cycles in systems directly connected to renewable generation. These findings outline key opportunities for future electrolyzer deployments and the synergistic benefits between electrolyzers and increased deployment of renewable energy generation like wind and solar. They also inform research and development that is reducing electrolyzer capital cost while managing durability impacts.

electricity markets↗
DOE OSTI2023

Verifying MCNP Models of the TEX High 240 Plutonium Benchmark

Computational modeling programs are invaluable tools that allow us to understand systems, safely develop new processes, and make reliable predictions about future designs. However, the effectiveness of these codes is limited by the degree to which their parameters match the real world. In the field of nuclear engineering, cross section data is one of these vital parameters. Accurate cross section data on important fissile and fissionable isotopes promotes the design of safer and more efficient fabrication, transportation, storage, and stockpiling of nuclear fuel. Unfortunately, there are knowledge gaps in data on key isotopes. In 2011, a multinational meeting hosted by the US Department of Energy Nuclear Criticality Safety Program ranked the priority of certain cross section data needs. In response, Lawrence Livermore National Lab (LLNL) designed the Thermal and Epithermal eXperiment (TEX) series of benchmark experiments. Benchmark experiments are used to validate current cross section data. They validate data by comparing the results of an actual experiment to the predicted results from a computational model. The data a benchmark applies to depends on the isotope and energy range the experiment’s neutron multiplication factor ( k eff ) is most sensitive to. The development and testing of the TEX High 240 Plutonium Benchmark will help validate 240 Pu cross section data. The configuration and materials of this benchmark are designed to be most sensitive to 240 Pu's intermediate energy range (from 0.625 ev to 100 keV ). MCNP® models of the assembly have been developed by LLNL and the results have been written in the final design report. In order for the discrepancies between benchmark models and experiments to be attributed to cross section inaccuracies, the accuracy of the models needs to be verified. The goal of this project is to verify of the results of LLNL's modeling by creating a new set of MCNP models and comparing the results.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Toward Quantum Chemical Free Energy Simulations of Platinum Nanoparticles on Titania Support

Platinum nanoparticles (Pt-NPs) supported on titania surfaces are costly but indispensable heterogeneous catalysts because of their highly effective and selective catalytic properties. Therefore, it is vital to understand their physicochemical processes during catalysis to optimize their use and to further develop better catalysts. However, simulating these dynamic processes is challenging due to the need for a reliable quantum chemical method to describe chemical bond breaking and bond formation during the processes but, at the same time, fast enough to sample a large number of configurations required to compute the corresponding free energy surfaces. Density functional theory (DFT) is often used to explore Pt-NPs; nonetheless, it is usually limited to some minimum-energy reaction pathways on static potential energy surfaces because of its high computational cost. In this work, we report a combination of the density functional tight binding (DFTB) method as a fast but reliable approximation to DFT, the steered molecular dynamics (SMD) technique, and the Jarzynski equality to construct free energy surfaces of the temperature-dependent diffusion and growth of platinum particles on a titania surface. In particular, we present the parametrization for Pt-X (X = Pt, Ti, or O) interactions in the framework of the second-order DFTB method, using a previous parametrization for titania as a basis. The optimized parameter set was used to simulate the surface diffusion of a single platinum atom (Pt 1 ) and the growth of Pt 6 from Pt 5 and Pt 1 on the rutile (110) surface at three different temperatures (T = 400, 600, 800 K). The free energy profile was constructed by using over a hundred SMD trajectories for each process. We found that increasing the temperature has a minimal effect on the formation free energy; nevertheless, it significantly reduces the free energy barrier of Pt atom migration on the TiO 2 surface and the transition state (TS) of its deposition. In a concluding remark, the methodology opens the pathway to quantum chemical free energy simulations of Pt-NPs’ temperature-dependent growth and other transformation processes on the titania support.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Entangled two-photon absorption with Brownian-oscillator fluctuations

Here, we theoretically investigate the two-photon absorption signals of a three-band (g, e, f) system diagonally coupled to an over-damped Brownian oscillator bath, which induces random Gaussian modulations of energy levels with an arbitrary degree of correlation. For fast modulation, extra 2ω eg and 2ω fe peaks may obscure the g–f transitions in the classical two-photon absorption (CTPA) spectra for nearly resonant e states. These peaks arise from one-photon resonant g–e or e–f transitions. In the slow modulation limit, these peaks vanish because of the short tails of the Gaussian line shape. CTPA strongly depends on the correlations between energy fluctuations. In entangled two-photon absorption, the extra peaks are eliminated because of the broad one-photon but narrow two-photon spectrum of the twin photons. The variation of the coherences between f states with the correlation between energy fluctuations is explored.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Acceleration of Oxygen Ions in Dipolarization Events: 1. CPS Distributions

Abstract Using an MHD simulation of near tail reconnection associated with a flow burst and the collapse (dipolarization) of the inner tail in combination with test particle tracing we study the acceleration and flux increases of energetic oxygen ions (O + ). The characteristic orbits, distributions, and acceleration mechanisms are governed by the dimensionless parameter σ = ω ci t n , where ω ci is the ion gyro frequency and t n a characteristic Alfvén time of the MHD simulation. For σ < 1, central plasma sheet (CPS) populations after the passage of the dipolarization front are found to resemble half‐shells in velocity space oriented toward dusk. They originate from within the CPS and are energized typically by a single encounter of the region of enhanced cross‐tail electric field associated with the flow burst. For larger σ values ( σ > 1) the O + distributions resemble more closely those of protons, consisting of two counter‐streaming field‐aligned beams and an, albeit more tenuous and irregular, ring population perpendicular to the magnetic field. The existence of the beams, however, depends on suitable earthward moving source populations in the plasma sheet boundary layer or the adjacent lobes. The acceleration to higher energies is found to indicate a charge dependence, consistent with a dominance of more highly charged ions at energies of a few hundred keV. As in earlier simulations, the simulated fluxes show large anisotropies and nongyrotropic effects, phase bunching, and spatially and temporally localized beams.

Birn, J.↗
DOE OSTI2021

Chapter 6: Economic Development: Renewables, Sustainable Economies, & Carbon Offsets

This chapter reviews economic development issues and opportunities that Tribes face in the age of climate change. It includes summaries pertaining to Tribal histories and trauma, harmful federal policies and subsequent land tenure issues, and the surge of economic sovereignty through renewable energy development on Tribal lands, including carbon offset markets. Recommendations are offered to reinforce and expedite Tribal economic self-determination on Tribal lands in the context of climate change. The chapter opens with the narrative of the Ute Mountain Ute Tribe of southwest Colorado, describing how this Tribe developed a large-scale solar economic development project to reduce their Tribal energy bills and decrease their dependence on fossil fuel usage. A researched overview of Economic Development as it relates to Tribes and climate change follows these narratives, beginning with the Key Messages and Recommendation that the authors have identified.

climate change↗
DOE OSTI2025

Cooper minima of atoms in a plasma environment

Recent efforts have extended the calculations of photon ionization and associated Cooper minima to atoms in a plasma environment simulated by screening the atomic potential. Furthermore, in this paper previously unrecognized features of bound electron photon excitations in screened atomic potentials are examined. First, the Cooper minima location as a function of photon energy is shown to be weakly dependent on the screening, which is explained by stationary perturbation theory. Second, the screening transfers transition probability from high to low photon energies relative to the isolated atom result.

Cooper minima↗
DOE OSTI2025

A machine learning method of modern urban building energy modeling: A case study of Chicago

Urban-scale building energy modeling is vital for urban planning. However, it can be challenging to assimilate reliable non-geometry building data for urban-scale modeling without extensive investment. Here, this study introduces a novel approach to developing modern urban-scale building energy stock data using geographic information systems and machine learning algorithms without necessarily requiring pre-supplied non-geometric metadata. The proposed framework integrates building footprint and height data to estimate gross floor areas, and matches each building to a pool of candidate records from ComStock or ResStock—filtered to the same county and ranked by geometric similarity—demonstrate a proof-of-concept case study in Chicago for predicting energy use intensity (EUI) using scalable datasets. The model achieved a mean bias error (MBE) of 0.08 kWh/m² and root mean square error (RMSE) of 14.84 kWh/m² under full metadata input for EUI prediction. With only location inputs, the model captured 69.2 % of EUI within predicted ranges. These results demonstrate the model’s potential to support early-stage urban planning, identify candidates for energy-efficient retrofits. By removing the dependency on detailed pre-surveys or extensive building metadata, the approach overcomes a key barrier in traditional urban-scale building energy modeling, illustrating a pathway toward broader and more cost-effective application, though further multi-city validation and improved treatment of pre-1925 buildings are needed.

Energy Use Intensity↗
DOE OSTI2021

Fast Emulation of Expensive Simulations using Approximate Gaussian Processes [Slides]

Nuclear Computational Low-Energy Initiative (NUCLEI) collaboration uses Density Functional Theory (DFT) simulations to predict the structure and binding energies of nuclei over a wide range of proton (Z) and neutron (N) numbers. The DFT simulations utilize a particular parameterization of a Skyrme energy density functional called UNEDF1 which depends on 12 free parameters that must be fit to data (M Kortelainen et al 2014). Fitting involves comparing (e.g.) predicted binding energies of nuclei to experimentally measured values. We use only binding energies as observables, but DFT with UNEDF1 will predict structure (shape) observables as well. In this work, assessing the capability of approximate GP emulators to balance emulator accuracy with computational speed to facilitate improved UNEDF1 calibration. Sparse GPs are straightforward to train and accurate. Calibration is not straightforward with MCMC (using MH or HMC/NUTS). We produced reusable software for continuing and building on this work as well as accessing and using Darwin cluster compute resources

97 MATHEMATICS AND COMPUTING↗