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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 955 records · Page 53
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

{beta}- and {gamma}-spectroscopy study of {sup 119}Pd and {sup 119}Ag

Neutron-rich Pd-119 nuclei were produced in fission of natural uranium, induced by 25-MeV protons. Fission fragments swiftly extracted with the Ion Guide Isotope Separation On-Line method were mass separated using a dipole magnet and a Penning trap, providing mono-isotopic samples of Pd-119. Their beta(-) decay was measured with gamma gamma- and beta gamma-spectroscopy methods using low-energy germanium detectors and a thin plastic scintillator. Two distinct nuclear-level structures were observed in Ag-119, based on the 1/2(-) and 7/2(+) isomers reported previously. The beta(-)decay work was complemented by a prompt-gamma study of levels in Ag-119 populated in spontaneous fission of (252)cf, performed using the Gammasphere array of germanium detectors. Contrary to previous suggestions, our data show that the 1/2(-) isomer is located below the 7/2(+) isomer and is proposed as a new ground state of Ag-119 with the 7/2(+) isomer excitation energy determined to be 33.4 keV. Our data indicate that there are two beta unstable isomers in Pd-119, a proposed ground state of Pd-119 with tentative spin 1/2(-) or 3/2(+) and a half-life of 0.88 s and the other one about 350 keV above, having spin (11/2(-)) and a half-life of 0.85 s. The higher-energy isomer probably decays to the 1/2(-) or 3/2(+) ground state via a gamma cascade comprising 18.7-219.8-X-keV transitions. The unobserved isomeric transition with energy X approximate to 100 keV probably has an E3 multipolarity. Its hindrance factor is significantly lower than for analogous E3 isomeric transitions in lighter Pd isotopes, suggesting an oblate deformation of levels in Pd-119. Oblate configurations in Ag-119 are discussed also.

Kurpeta, J↗
DOE OSTI2024

Physics-assisted Latent Space Dynamics Learning for Stiff Collisional-radiative Models

Collisional-radiative (CR) models describe the atomic processes in a plasma by tracking the population density in the ground and excited states for each charge state of the atom/ion. These models predict important plasma properties such as charge state distributions and radiative emissivity and opacity. Accurate descriptions of the CR balance of the plasma are essential in fusion whole device modeling, especially when significant impurities are introduced into the plasmas. In an integrated fusion plasma and CR simulation, a CR model, which is a high-dimensional stiff ODE, needs to be solved on each grid point in the configuration space, and can overwhelm the overall computational cost. In this work, we propose a machine-learning-based method that discovers a latent space and learns its corresponding latent dynamics, which can capture the essential physics to make accurate predictions at much lower online computational cost. The proposed approach is physics-assisted, due to its combination of a physical latent space and a data-driven latent space. It has been demonstrated that the proposed architecture can predict both the full-order CR dynamics and a physical quantity of interest accurately.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Simultaneous estimation of multiple eigenvalues with short-depth quantum circuit on early fault-tolerant quantum computers

We introduce a multi-modal, multi-level quantum complex exponential least squares (MM-QCELS) method to simultaneously estimate multiple eigenvalues of a quantum Hamiltonian on early fault-tolerant quantum computers. Our theoretical analysis demonstrates that the algorithm exhibits Heisenberg-limited scaling in terms of circuit depth and total cost. Notably, the proposed quantum circuit utilizes just one ancilla qubit, and with appropriate initial state conditions, it achieves significantly shorter circuit depths compared to circuits based on quantum phase estimation (QPE). Numerical results suggest that compared to QPE, the circuit depth can be reduced by around two orders of magnitude under several settings for estimating ground-state and excited-state energies of certain quantum systems.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2023

Nonlinear Impact-Echo Test for Quantitative Evaluation of ASR Damage in Concrete

Nonlinear acoustic methods demonstrate high sensitivity for concrete damage evaluation. Among these methods, nonlinear resonance acoustic methods have been widely used in laboratory tests on small scale test samples. In this study, a nonlinear impact-echo (IE) method for concrete damage evaluation was introduced, in which the IE frequency shift was measured at different impact force levels. The nonlinear IE test and the nonlinear impact resonance acoustic spectroscopy (NIRAS) test share similarities in the experimental setup and analysis method. However, the nonlinear IE test excites a local thickness resonance mode of a member instead of the global resonance vibration. Therefore, the analyzed mode is unaffected by member boundary conditions and is applicable to large concrete structural members. To identify the fundamental IE frequencies, multiple impacts were applied along the members. Once the fundamental IE frequencies were determined, the effectiveness of the nonlinear IE method was evaluated by testing seven concrete beam specimens with varying levels of alkali-silica reaction (ASR) damage. In conclusion, the nonlinear IE test demonstrates high sensitivity to concrete damage and allows for quantitative assessment of the damage state of concrete without a baseline measurement.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Quantum solver for single-impurity Anderson models with particle-hole symmetry

Quantum embedding methods, such as dynamical mean-field theory (DMFT), provide a powerful framework for investigating strongly correlated materials. A central computational bottleneck in DMFT is in solving the Anderson impurity model (AIM), whose exact solution is classically intractable for large bath sizes. In this work, we benchmark a quantum-classical hybrid solver tailored for particle-hole symmetric AIMs, using the variational quantum eigensolver to prepare the ground state of the model with shallow quantum circuits. The solver uses shallow quantum ansätze and one set of variational parameters to prepare the ground state and its particle and hole excitations, enabling the construction of the impurity Green’s function through a continued-fraction expansion. We evaluate the performance of this approach across a few bath sizes and interaction strengths under noisy, shot-limited conditions. We compare three optimization routines (COBYLA, Adam, and L-BFGS-B) in terms of convergence and fidelity, assess the benefits of estimating a quantum-computed moment correction to the variational energies, and benchmark the approach by comparing the density of states computed from the impurity Green’s function against that obtained using a classical pipeline. Our results demonstrate the feasibility of Green’s function construction on near-term devices and establish practical benchmarks for quantum impurity solvers embedded within self-consistent DMFT loops.

Karabin, Mariia [ORNL]↗
NASA NTRS2004

Computation of Gust-Cascade Interaction Using the CE/SE Method

The problem 2 in Category 3 of the 4th Computational Aeroacoustic(CAA) Workshop is solved using the space-time conservation element and solution element (CE/SE) method. This problem models rotor-stator interaction in a 2D cascade. It involves complex geometries and flow physics including vortex shedding and acoustic radiation. The parallel version of the 2D nonlinear Euler solver is used with an unstructured triangular mesh to solve this problem. The Giles approach is incorporated with the CE/SE method to handle non-equal pitches of the rotor and stator. Validation on the Giles approach is performed using Problem 3.1 in the 2nd CAA Workshop. The space-time CE/SE method is a finite volume method with second-order accuracy in both space and time. The flux conservation is enforced in both space and time instead of space only. It has low numerical dissipation and dispersion errors. It uses simple non-reflecting boundary conditions and is compatible with unstructured meshes. It is simple, flexible, and generate reasonably accurate solutions. The CE/SE method has been successfully applied to solve numerous practical problems, especially aeroacoustic problems. Some preliminary numerical results of the benchmark problem 3.2 of the 4th CAA Workshop are shown. The steady-state pressure contour is plotted. The mean pressure distribution on the blade surface is compared with Turbo solution showing a good agreement. The sound pressure level versus the rotor harmonic n at the six designated positions on the blade surface, three locations at inlet plane, and three locations at the outlet plane are plotted. It can be seen that the acoustic response exists only at the excitation frequencies (n = 1,2,3). On the blade surface, the acoustic wave at n = 1 is dominant, while at the inlet and outlet planes, the sound pressure level at n = 2 becomes the largest, which is similar to the results presented. The distribution of sound pressure level at different spatial modes along the z- direction is plotted for n = 1,2,3, respectively. It shows that the spatial modes m = -32 and 22 at n = 1 exponentially decay, and the spatial modes m = 10 at n = 2, m = -42 and 12 at n = 3 propagate both upstream and downstream, which agrees with the prediction based on the linearized theory. Some oscillations are observed, which needs to be investigated further. In the final paper, the numerical results will be compared with a frequency-domain solver LINFLUX solution if it is available.

Wang, X.-Y.↗
NASA NTRS1989

Method for producing an atomic oxygen beam

A method for producing an atomic oxygen beam is provided by the present invention. First, a material 10' is provided which dissociates molecular oxygen and dissolves atomic oxygen into its bulk. Next, molecular oxygen is exposed to entrance surface 11' of material 10'. Next, material 10' is heated by heater 17' to facilitate the permeation of atomic oxygen through material 10' to the UHV side 12'. UHV side 12' is interfaced with an ultra-high vacuum (UHV) environment provided by UHV pump 15'. The atomic oxygen on the UHV side 12' is excited to a non-binding state by exciter 14' thus producing the release of atomic oxygen to form an atomic oxygen beam 35'.

Outlaw, Ronald A.↗
DOE OSTI2021

Non-intrusive nonlinear model reduction via machine learning approximations to low-dimensional operators

Abstract Although projection-based reduced-order models (ROMs) for parameterized nonlinear dynamical systems have demonstrated exciting results across a range of applications, their broad adoption has been limited by their intrusivity: implementing such a reduced-order model typically requires significant modifications to the underlying simulation code. To address this, we propose a method that enables traditionally intrusive reduced-order models to be accurately approximated in a non-intrusive manner. Specifically, the approach approximates the low-dimensional operators associated with projection-based reduced-order models (ROMs) using modern machine-learning regression techniques. The only requirement of the simulation code is the ability to export the velocity given the state and parameters; this functionality is used to train the approximated low-dimensional operators. In addition to enabling nonintrusivity, we demonstrate that the approach also leads to very low computational complexity, achieving up to $$10^3{\times }$$ 10 3 × in run time. We demonstrate the effectiveness of the proposed technique on two types of PDEs. The domain of applications include both parabolic and hyperbolic PDEs, regardless of the dimension of full-order models (FOMs).

42 ENGINEERING↗
NASA NTRS1996

A correlated ab initio study of the X2A1 and A2E states of MgCH3

The X2A1 and A2E states of the MgCH3 radical have been studied with correlation consistent basis sets and the coupled cluster method RCCSD(T) in order to compare with two recent experimental efforts [M. A. Anderson and L. M. Ziurys, Astrophys. J. 452, L157 (1995); R. Rubino, J. M. Williamson, and T. A. Miller, J. Chem. Phys. 103, 5964 (1995)]. The best computed values [RCCSD(T)/cc-pCVTZ] for the X2A1 state are (experimental results in parentheses): Ae = 160.433 GHz, Be = 10.948 GHz (B0 = 11.008 GHz), and Mue = 1.011 D. The Mg-CH3 bond is weak, 26.3 kcal/mol. Values for the A2E state are Ae = 154.648 GHz (A0 = 149.666 GHz), Be = 10.87 GHz (B0 = 10.932 GHz), and Mue = 1.022 D. The excitation energy (Te) for the A2E <-- X2A1 transition is 19 999 cm-1 (T00 = 20 030 cm-1). A brief discussion of bonding trends in Mg-containing radials is included.

Non-NASA Center↗
DOE OSTI2022

Scalable Deep Learning-Based Microarchitecture Simulation on GPUs

Cycle-accurate microarchitecture simulators are essential tools for designers to architect, estimate, optimize, and manufacture new processors that meet specific design expectations. However, conventional simulators based on discrete-event methods often require an exceedingly long time-to-solution for the simulation of applications and architectures at full complexity and scale. Given the excitement around wielding the machine learning (ML) hammer to tackle various architecture problems, there have been attempts to employ ML to perform architecture simulations, such as Ithemal and SimNet. However, the direct application of existing ML approaches to architecture simulation may be even slower due to overwhelming memory traffic and stringent sequential computation logic. This work proposes the first graphics processing unit (GPU)-based microarchitecture simulator that fully unleashes the potential of GPUs to accelerate state-of-the-art ML-based simulators. First, considering the application traces are loaded from central processing unit (CPU) to GPU for simulation, we introduce various designs to reduce the data movement cost between CPUs and GPUs. Second, we propose a parallel simulation paradigm that partitions the application trace into sub-traces to simulate them in parallel with rigorous error analysis and effective error correction mechanisms. Combined, this scalable GPU-based simulator outperforms by orders of magnitude the traditional CPU-based simulators and the state-of-the-art ML-based simulators, i.e., SimNet and Ithemal.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2021

Lattice collective modes from a continuum model of magic-angle twisted bilayer graphene

Here, we show that the insulating states of magic-angle twisted bilayer graphene support a series of collective modes corresponding to local particle-hole excitations on triangular lattice sites. Our theory is based on a continuum model of the magic angle flat bands. When the system is insulating at moiré band filling ν = -3, our calculations show that the ground state supports seven low-energy modes that lie well below the charge gap throughout the moiré Brillouin zone, one of which couples strongly to THz photons. The low-energy collective modes are faithfully described by a model with a local SU(8) degree of freedom in each moiré unit cell that we identify as the direct product of spin, valley, and an orbital pseudospin. Apart from spin and valley-wave modes, the collective mode spectrum includes a low-energy intraflavor exciton mode associated with transitions between flat valence and conduction band orbitals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Path Integral Monte Carlo Simulations of Iron Plasmas (Final Technical Report)

This documents is the final technical report for our grant entitled "Path Integral Monte Carlo Simulations of Iron Plasmas" that focused on developing path integral Monte Carlo (PIMC) computer simulations. This techniques will be developed to study plasmas composed of heavier elements including iron and other third row elements. Equations of state (EOS) and transport properties will be derived in the regime of warm dense matter (WDM) and dense plasmas where existing first-principles methods cannot be applied. While standard density functional theory (DFT) has been used to accurately predict the structure of many solids and liquids up to temperatures on the order of 100,000 K, this method is not applicable at much higher temperature because the number of partially occupied electronic orbitals reaches intractably large numbers or the use of finite-temperature free energy functionals in orbital-free DFT introduces an uncontrolled approximation. Here we focus on PIMC methods that become more and more efficient with increasing temperatures and still include all electronic correlation effects. In this approach, electronic excitations increase the efficiency rather than reduce it. While it had commonly been assumed this method could only be applied to elements without core electrons, we showed that PIMC with free-particle nodes works well for first-row elements (PRL 108 (2012) 115502). Most recently, we extended the applicability range of all-electron PIMC to second-row elements by adopting localized nodal surfaces (PRL 115 (2015) 176403). To simulate third-row elements efficiently under WDM conditions, we propose a new method to remove core electrons by introducing pseudo-nodes. We explain our approach step by step and present preliminary results. We focus our method development on getting PIMC simulations of iron to work because of its fundamental importance for WDM and astrophysics. Then we move on to krypton and copper-doped beryllium, a ICF ablator material. We plan to continue working on key second-row material such as Na, Mg, MgO, Al, silica, and silicon-doped plastic ablators. Our collaborators at LLNL, will use our PIMC EOS data both as comparisons to existing semi-empirical, EOS-generating schemes, and as input for continuum radiation hydrodynamics simulations. We will establish an efficient pipeline from PIMC to macroscopic continuum studies of materials response. An emphasis will be placed on benchmarking such methods for plasmas of heavy elements at the very high temperatures (~100 eV) and low densities that are generated when Hohlraum radiation heats the ablator material in indirect drive laser experiments. Results from changes to the EOS will be of immeasurable importance to the designers at the National Ignition Facility (NIF) and at other facilities. Starting with our EOS of Cu-doped Be, our second collaborator at LLE, will perform real-time simulations of laser fusion experiments at the Omega laser and at the NIF to determine how sensitive the compression path depends on the ablator EOS. Since our collaborator also has experience in performing orbital-free DFT calculations, we propose to compare predictions from this method with PIMC results. In joint publications, we plan to analyze the accuracy of different free-energy functionals in order to understand why existing orbital-free DFT calculations do not predict compression peaks along the shock Hugoniot curve that we see with PIMC. The peaks are caused by the ionization of various electron shells. Their accurate characterization is important to compare with experimental results. We will break new ground by developing PIMC techniques that can simulate iron and all other third row elements in the plasma and WDM regimes. We introduce the concept of pseudo-nodes for the efficient treatment of the core-electrons. The EOS and transport properties will be derived and published online in the form of a new WDM database. Our PIMC EOS calculations will benchmark and possibly replace semi-analytical EOS tables like QEOS or SESAME, which will impact the hydrocode simulation community and will affect the design of NIF targets. Our PIMC results will help to improve the accuracy of orbital-free DFT simulations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Phenylene-linked tetrapyrrole arrays containing free base and diverse metal chelate forms – Versatile synthetic architectures for catalysis and artificial photosynthesis

Tetrapyrrole macrocycles are central to photosynthesis yet a single macrocycle does not carry out photosynthesis; rather, assemblies of tetrapyrrole macrocycles work in concert in antenna complexes, reaction centers, and electron-transport chains to harvest sunlight, funnel excited-state energy and separate charge for biological use. A longstanding theme in artificial photosynthesis has been to construct covalently linked “arrays” of metalated and free base tetrapyrrole macrocycles for fundamental studies of such processes, which entail excited-state and ground-state interactions. Among linkers in arrays chemistry, the 1,2-, 1,3-, or 1,4-disubstituted phenylene unit has proved very attractive owing to the resulting short distance, defined architecture, and appropriate extent of electronic coupling of adjacent macrocycles to give rapid electron and/or energy transfer while largely retaining desired spectral features. Eight distinct strategies to construct phenylene-linked tetrapyrrole arrays are identified in a review with comprehensive coverage since inception in the early 1970s through mid-year 2021. The arrays predominantly incorporate porphyrins with very few chlorins and bacteriochlorins, reflecting historic availability of synthetic methods for macrocycle formation. Of the eight strategies, only two appear applicable to (bacterio)chlorins. While studies in artificial photosynthesis have largely fueled this field, applications in catalysis have also been examined. Altogether >400 arrays are covered. The review delves into synthesis and molecular design, sketches photophysical properties, and suggests unrealized opportunities in arrays chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Characterization of Deformational Isomerization Potential and Interconversion Dynamics with Ultrafast X-ray Solution Scattering

Dimeric complexes composed of d 8 square planar metal centers and rigid bridging ligands provide model systems to understand the interplay between attractive dispersion forces and steric strain in order to assist the development of reliable methods to model metal dimer complexes more broadly. [Ir 2 (dimen) 4 ] 2+ (dimen = para-diisocyanomenthane) presents a unique case study for such phenomena, as distortions of the optimal structure of a ligand with limited conformational flexibility counteract the attractive dispersive forces from the metal and ligand to yield a complex with two ground state deformational isomers. Here, in this work, we use ultrafast X-ray solution scattering (XSS) and optical transient absorption spectroscopy (OTAS) to reveal the nature of the equilibrium distribution and the exchange rate between the deformational isomers. The two ground state isomers have spectrally distinct electronic excitations that enable the selective excitation of one isomer or the other using a femtosecond duration pulse of visible light. We then track the dynamics of the nonequilibrium depletion of the electronic ground state population—often termed the ground state hole—with ultrafast XSS and OTAS, revealing a restoration of the ground state equilibrium in 2.3 ps. This combined experimental and theoretical study provides a critical test of various density functional approximations in the description of bridged d 8 –d 8 metal complexes. The results show that density functional theory calculations can reproduce the primary experimental observations if dispersion interactions are added, and a hybrid functional, which includes exact exchange, is used.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Isospin 0 and 2 two-pion scattering at physical pion mass using all-to-all propagators with periodic boundary conditions in lattice QCD

A study of two-pion scattering for the isospin channels, 𝐼 = 0 and 𝐼 = 2, using lattice QCD is presented. Möbius domain-wall fermions, on top of the Iwasaki-DSDR gauge action for gluons with periodic boundary conditions, are used for the lattice computations, which are carried out on two ensembles of gauge field configurations generated by the RBC and UKQCD Collaborations with physical masses, inverse lattice spacings of 1.023 and 1.378 GeV, and spatial extents of 𝐿 = 4.63 and 4.58 fm, respectively. The all-to-all propagator method is employed to compute a matrix of correlation functions of two-pion operators. The generalized eigenvalue problem (GEVP) is solved for a matrix of correlation functions to extract phase shifts with multiple states—two pions with a nonzero relative momentum, as well as two pions at rest. Our results for phase shifts for both the 𝐼 = 0 and 𝐼 = 2 channels are consistent with the Roy equation and chiral perturbation theory, though at this preliminary stage our errors for 𝐼 = 0 are large. An important outcome of this work is that we are successful in extracting two-pion excited states, which are useful for studying 𝐾 → 𝜋⁢𝜋 decay, on physical-mass ensembles using the GEVP.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
NASA NTRS2018

Planetary Spectrum Generator: An Accurate Online Radiative Transfer Suite for Atmospheres, Comets, Small Bodies and Exoplanets

We have developed an online radiative-transfer suite (https://psg.gsfc.nasa.gov) applicable to a broad range of planetary objects (e.g., planets, moons, comets, asteroids, TNOs, KBOs, exoplanets). The Planetary Spectrum Generator (PSG) can synthesize planetary spectra (atmospheres and surfaces) for a broad range of wavelengths (UV/Vis/near-IR/IR/far-IR/THz/sub-mm/Radio) from any observatory (e.g., JWST, ALMA, Keck, SOFIA), any orbiter (e.g., ExoMars, Juno), or any lander (e.g., MSL). This is achieved by combining several state-of-the-art radiative transfer models, spectroscopic databases and planetary databases (i.e., climatological and orbital). PSG has a 3D (three-dimensional) orbital calculator for most bodies in the solar system, and all confirmed exoplanets, while the radiative-transfer models can ingest billions of spectral signatures for hundreds of species from several spectroscopic repositories. It integrates the latest radiative-transfer and scattering methods in order to compute high resolution spectra via line-by-line calculations, and utilizes the efficient correlated-k method at moderate resolutions, while for computing cometary spectra, PSG handles non-LTE and LTE excitation processes. PSG includes a realistic noise calculator that integrates several telescope/instrument configurations (e.g., interferometry, coronagraphs) and detector technologies (e.g., CCD, heterodyne detectors, bolometers). Such an integration of advanced spectroscopic methods into an online tool can greatly serve the planetary community, ultimately enabling the retrieval of planetary parameters from remote sensing data, efficient mission planning strategies, interpretation of current and future planetary data, calibration of spectroscopic data, and development of new instrument/spacecraft concepts.

Villanueva, G. L.↗
DOE OSTI2024

Solid State Reduction Driven Synthesis of Mn Containing Multi-principal Component Alloys

In recent years, high entropy alloys (HEAs), also known as multi-principal component alloys (MPCAs) have emerged as a new and exciting class of materials. This paper reports on the solid state reduction synthesis of a series of CoFeNiMn-based MPCA compositions, starting from a mixture of the corresponding oxides. One of the aims of the study was to test whether the degree of reduction of MnO, a highly stable oxide, could be enhanced by tailoring the alloy composition. Specifically, the influence of Ni content was studied because Ni exhibits a significant negative enthalpy of mixing with Mn. High purity precursor powders of Co(OH) 2 , Fe 2 O 3 , MnO 2 , and NiO were milled and mixed using standard ceramic processing methods. Here, the nominal sample compositions (assuming complete oxide reduction) were (CoFeMn) x Ni (1-x) , for x = 0, 0.083, 0.166, and 0.25. The oxide samples were subjected to a series of isothermal reduction anneals in flowing 3 pct H 2 –Ar at 1100 °C. The resulting microstructures were characterized using scanning electron microscopy (SEM), X-ray energy dispersive spectroscopy (EDS) and X-ray diffraction (XRD). The composition of the resulting MPCAs was determined quantitatively using wavelength dispersive spectroscopy (WDS) in the electron microprobe. The study revealed that for each of the initial oxide compositions studied, it was possible to achieve an MPCA with ~ 25 at. pct Mn. These results were found to be consistent with the predictions of a thermodynamic model whereby a negative enthalpy of mixing (ΔH mix ), combined with a contribution from configurational entropy, can offset a positive free energy of reduction (ΔG red ). The incorporation of vibrational entropy into first principles calculations was found to have a significant effect on the predicted crystal structure of the MPCAs.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Atomic-Site-Specific Surface Valence-Band Structure from X-Ray Standing-Wave Excited Photoemission

X-ray standing-wave (XSW) excited photoelectron emission was used to measure the site-specific valence band (VB) for ½ monolayer (ML) Pt grown on a SrTiO 3 (001) surface. The XSW induced modulations in the core level (CL), and VB photoemission from the surface and substrate atoms were monitored for three ℎ⁡kl substrate Bragg reflections. The XSW CL analysis shows the Pt to have a face-centered-cubic-like cube-on-cube epitaxy with the substrate. The XSW VB information compares well to a density functional theory calculated projected density of states from the surface and substrate atoms. Altogether, this Letter represents a novel method for determining the contribution to the density of states by valence electrons from specific atomic surface sites.

74 ATOMIC AND MOLECULAR PHYSICS↗