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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 379 records · Page 21
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Itinerant G-type antiferromagnet SrCr 2 As 2 studied by magnetization, heat capacity, electrical resistivity, and NMR measurements

Here, the physical properties of itinerant antiferromagnetic (AFM) SrCr 2 As 2 with body-centered tetragonal ThCr 2 Si 2 structure were investigated in single crystalline and polycrystalline forms by electrical resistivity ρ, heat capacity C p , magnetic susceptibility χ versus temperature T, and magnetization M versus applied magnetic field H isotherm measurements as well as 75 As and 53 Cr nuclear magnetic resonance (NMR) measurements in the wide temperature range T = 1.6–900 K. From the χ(T) and 75 As NMR measurements, the G-type AFM state below T N = 615(15) K has been determined, consistent with the previous neutron-diffraction measurements. Direct evidence of magnetic ordering of the Cr spins was shown by the observation of the 53 Cr NMR spectrum under H = 0. From the χ( T) measurements on single-crystal SrCr 2 As 2 under the two different magnetic field directions H|| ab and H || c in the AFM state, the Cr ordered moments are shown to align along the c axis in the G-type AFM state. The metallic state is directly evidenced by the ρ, C p , and NMR measurements, and the density of states at the Fermi energy $\mathscr{D}$(E F ) in the AFM state is estimated to be 7.53 states/eV f.u. for both spin directions which is almost twice the bare $\mathscr{D}$(E F ) estimated from first-principles calculations, suggesting an enhancement of the conduction-carrier mass by a factor of two in the AFM state. The $\mathscr{D}$(E F ) is found to be nearly constant below at least 100 K and is independent of H. The ρ(T) is found to show T-linear behavior above T N and exhibits positive curvature below T N where significant loss of spin-disorder scattering upon magnetic ordering is observed. The resistivity anisotropy of the compound remains moderate ρ c /ρ a ~ 9 through most of the magnetically ordered phase but shows a rapid increase below 50 K.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Itinerant ferromagnetism and intrinsic anomalous Hall effect in amorphous iron-germanium

The amorphous iron-germanium system ( a - Fe x Ge 1 - x ) lacks long-range structural order and hence lacks a significant Brillouin zone. The magnetization of a - Fe x Ge 1 - x is well explained by the Stoner model for Fe concentrations x above the onset of magnetic order around x = 0.4 , indicating that the local order of the amorphous structure preserves the spin-split density of states of the Fe- 3 d states sufficiently to polarize the electronic structure despite k being a bad quantum number. Measurements reveal an enhanced anomalous Hall resistivity ρ x y AH relative to crystalline FeGe; this ρ x y AH is compared to density-functional theory calculations of the anomalous Hall conductivity to resolve its underlying mechanisms. The intrinsic mechanism, typically understood as the Berry curvature integrated over occupied k states but shown here to be equivalent to the density of curvature integrated over occupied energies in aperiodic materials, dominates the anomalous Hall conductivity of a - Fe x Ge 1 - x ( 0.38 ≤ x ≤ 0.61 ). The density of curvature is the sum of spin-orbit correlations of local orbital states and can hence be calculated with no reference to k space. This effect and the accompanying Stoner-like model for the intrinsic anomalous Hall conductivity establish a unified understanding of the underlying physics of the anomalous Hall effect in both crystalline and disordered systems.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Computational search for itinerant n -type and p -type magnetic semiconductors: Arsenopyrites as bipolar magnetic semiconductors

We report a computational search for three-dimensional bulk ferromagnetic semiconductors based on itinerant Stoner physics. Stoner-based ferromagnetic semiconductors require an unusual combination of high band edge density of states and moderate transport effective mass. Nonetheless, several potential materials are found. Here, we identify arsenopyrites, exemplified by FeAsS, as materials that, with suitable doping, exhibit ferromagnetic semiconducting behavior for both n- and p-type dopants. The existence of a material that becomes ferromagnetic for both p and n types may enable device concepts, for example, ferromagnetic p–n junction devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Increased Voltage in CdSe Solar Cells by Mitigation of Charge Carrier Trapping Due to Se Vacancies

Cadmium selenide (CdSe), with a 1.7 eV bandgap, is a promising high-bandgap semiconductor for tandem solar cells, yet device efficiencies are hindered by rapid minority carrier recombination. Here, in this study, polycrystalline CdSe solar cells are investigated using radiative emission spectroscopy, time-resolved photoluminescence, and density functional theory, revealing fast (sub-nanosecond) minority carrier trapping by selenium vacancy-related defect states with densities of (5–50) × 10 17 cm −3 , limiting carrier mobility and increasing recombination. By reducing absorber thickness to ≈0.5 µm, trapping effects are mitigated, achieving a record open-circuit voltage of 917 mV, a 165 mV improvement over prior reports. These findings clarify the role of Se vacancies in limiting CdSe solar cell performance and provide insights applicable to CdSe and CdSeTe thin-film photovoltaics. This work advances understanding of defect-mediated losses in II–VI semiconductors and suggests pathways for improving solar cell performance through defect control.

14 SOLAR ENERGY↗
DOE OSTI2023

Electronic structure of boron and aluminum δ -doped layers in silicon

Recent work on atomic-precision dopant incorporation technologies has led to the creation of both boron and aluminum δ-doped layers in silicon with densities above the solid solubility limit. For this study, we use density functional theory to predict the band structure and effective mass values of such δ layers, first modeling them as ordered supercells. Structural relaxation is found to have a significant impact on the impurity band energies and effective masses of the boron layers, but not the aluminum layers. However, disorder in the δ layers is found to lead to a significant flattening of the bands in both cases. We calculate the local density of states and doping potential for these δ-doped layers, demonstrating that their influence is highly localized with spatial extents at most 4 nm. We conclude that acceptor δ-doped layers exhibit different electronic structure features dependent on both the dopant atom and spatial ordering. This suggests prospects for controlling the electronic properties of these layers if the local details of the incorporation chemistry can be fine-tuned.

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

Excess heat capacity in magnetically ordered Ce heavy-fermion metals

Herein we study the magnetic heat capacity of a series of magnetically ordered Ce-based heavy-fermion materials, which show an anomalous T 3 heat capacity in excess of the phonon contribution in many materials. For compounds for which magnon models have been worked out, we show that the local-moment magnon heat capacity derived from the measured magnon spectra underestimates the experimental specific heat. The excess heat capacity reveals increasing density of states with increasing energy, akin to a pseudogap. We show that this anomalous temperature-dependent term is not associated with proximity to a quantum critical point, but is strongly correlated with T N , indicating the anomalous excitations are governed by the magnetic exchange interaction. This insight may hold key information for understanding magnetically ordered heavy fermions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Compositionally Complex Alloys: Some Insights from Photoemission Spectroscopy

Photoemission spectroscopy (PES) is an underrepresented part of current and past studies of compositionally complex alloys (CCA) such as high-entropy alloys (HEA) and their derivatives. PES studies are very important for understanding the electronic structure of materials, and are therefore essential in some cases for a correct description of the intrinsic properties of CCAs. Here, we present several examples showing the importance of PES. First, we show how the difference between the split-band structure and the common-band structure of the valence band (VB), observed by PES, can explain a range of properties of CCAs and alloys in general. A simple description of the band crossing in CCAs composed from the early and late transition metals showing a split band is discussed. We also demonstrate how a high-accuracy PES study can determine the variation in the density of states at the Fermi level as a function of Cu content in Ti-Zr-Nb-Ni-Cu metallic glasses. Finally, the first results of an attempt to single out the contributions of particular constituents in Cantor-type alloys to their VBs are presented. The basic principles of PES, the techniques employed in studies presented, and some issues associated with PES measurements are also described.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Electromagnetic Properties of Aluminum-based Bilayers for Kinetic Inductance Detectors

The complex conductivity of a superconducting thin film is related to the quasiparticle density, which depends on the physical temperature and can also be modified by external pair breaking with photons and phonons. This relationship forms the underlying operating principle of Kinetic Inductance Detectors (KIDs), where the detection threshold is governed by the superconducting energy gap. We investigate the electromagnetic properties of thin-film aluminum that is proximitized with either a normal metal layer of copper or a superconducting layer with a lower T-C, such as iridium, in order to extend the operating range of KIDs. Using the Usadel equations along with the Nam expressions for complex conductivity, we calculate the density of states and the complex conductivity of the resulting bilayers to understand the dependence of the pair breaking threshold, surface impedance, and intrinsic quality factor of superconducting bilayers on the relative film thicknesses. The calculations and analyses provide theoretical insights in designing aluminum-based bilayer kinetic inductance detectors for detection of microwave photons and athermal phonons at the frequencies well below the pair breaking threshold of a pure aluminum film.

complex conductivity↗
DOE OSTI2023

Out-of-equilibrium Majorana zero modes in interacting Kitaev chains

Here, we employ a time-dependent real-space local density-of-states method to study the movement and fusion of Majorana zero modes in the one-dimensional interacting Kitaev model, based on the time evolution of many-body states. We analyze the dynamics and both fusion channels of Majoranas using time-dependent potentials, either creating walls or wells. For fast moving Majoranas, we unveil nonequilibrium signatures of the “strong-zero-mode” operator (quasiparity degeneracy in the full spectrum) and its breakdown in the presence of repulsive Coulomb interactions. Focusing on forming a full electron after fusion, we also discuss the upper and lower limits on the Majorana speed needed to reduce nonadiabatic effects and to avoid poisoning due to decoherence.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

First-principles investigation of uranium mononitride (UN): Effect of magnetic ordering, spin-orbit interactions and exchange correlation functional

Uranium mononitride (UN) is a promising nuclear fuel that combines the advantageous properties of readily used UO 2 and uranium alloys. Various properties of UN have been previously studied using different density functional theory (DFT) methodologies; however, there are still inconsistencies when it comes to the dynamical stability and defect properties of UN. We address these inconsistencies by studying the UN phonons and defect properties using DFT calculations employing two generalized gradient approximation (GGA) exchange-correlation functionals: PBE and AM05, with and without an added on-site Coulomb repulsion term (+U). Furthermore, we investigate the importance of spin-orbit coupling (SOC) when calculating the properties of UN. We use the different methodologies to determine the preference of UN to have antiferromagnetic (AFM) ordering, as seen in experiments, or ferromagnetic (FM) ordering of the uranium spins. We compare the crystallographic properties, density of states, the DFT X-ray photoelectron spectra and phonon dispersions calculated using the different methodologies. We demonstrate that GGA + U reproduces the AFM ordering in UN, but the crystal structure is dynamically unstable. We also show that magnetic ordering is important in finding the lowest energy defective structure, and that SOC has a distinct influence on the energy of the different uranium interstitial defects. Lastly, we discuss the point defect formation energies under U-rich and N-rich conditions, and the stoichiometric formation energies calculated with the different methodologies, providing insight into the observed tendency for forming hypostoichiometric UN.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Electronic structure of nitrogen-doped lutetium hydrides

First-principles density functional theory (DFT) calculations of supercell structures based on N-doped Fm $\bar3$m LuH 3 reveal configurations of Fm $\bar3$m Lu 8 H 23–x N that exhibit novel electronic properties such as flat bands, sharply peaked densities of states (van Hove singularities, vHs), and intersecting Dirac cones near the Fermi energy (E F ). These electronic properties are present when N substitutes H in the octahedral interstices of Fm $\bar3$ m LuH 3 . These structures also exhibit an interconnected metallic hydrogen network, a common feature of high-T c hydride superconductors. Electronic property systematics gives an estimate of T c for one structure that is well above the critical temperatures predicted for structures considered previously. DFT + U has an especially strong effect on one of the structures considered, enhancing the vHs and flat bands near E F . Finally, these results provide a basis for understanding the electronic properties observed for nitrogen-doped lutetium hydride.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Room temperature sodium diffusion in sodium iron phosphate investigated with neutron scattering

Sodium iron phosphate, Na x FePO 4 , is currently one of the most promising cathode materials for sodium ion batteries. Here we employ a systematic approach using three neutron scattering techniques to investigate temperature dependent properties with a focus on the charge transfer processes. Two distinct Na + diffusive motions are observed with quasielastic neutron scattering, including room temperature motion. These processes correspond to rapid double jumps through extrinsic vacancy sites of ∼6 Å along with the more fundamental nearest neighbor jumps of 3.1 Å. Experimental observations of room temperature ionic diffusion are highly desirable, as the diffusion pathways are naturally well suited for efficient transport. Inelastic neutron scattering was used to probe the vibrational density of states that assist in the ionic and electronic (polaronic) transport processes, which are further supported with density functional theory. Neutron diffraction examines the disordering of the sodium sublattice upon transition to the solid-solution phase, which is believed to enhance the overall kinetics during sodium insertion/extraction. Finally, 57 Fe Mössbauer spectroscopy measurements probes polaron hopping and the local structural evolution that modifies the electron density surrounding the redox active iron sites. This study sheds light on the temperature induced atomic scale dynamics that occur in olivine Na x FePO 4 .

Novak, Eric [Swarthmore College, Swarthmore, PA (U↗
DOE OSTI2024

First-Principles Calculations of the Electrical Conductivity of Carbon Nanotubes Functionalized with Copper and Nitrogen: Implications for Electronics, Energy Storage, and Nanodevices

In this work, we investigate the electrical conductivity of carbon nanotubes (CNTs), with a particular focus on the effects of doping. Using first-principles-based approaches, we study the electronic structure, phonon dispersion, and electron–phonon scattering to understand the finite-temperature electrical transport properties in CNTs. Our study covers both prototypical metallic and semiconducting CNTs, with special emphasis on the influence of typical defects such as vacancies and the incorporation of copper or nitrogen, such as pyridinic N, pyrrolic N, graphitic N, and oxidized N. Our theoretical study shows significant improvements in the electrical conduction properties of copper-CNT composites, especially when semiconducting CNTs are functionalized with nitrogen. Doping is found to cause significant changes in the electronic density of states near the Fermi level, which affects the electrical conductivity. Calculations show that certain types of functional groups, such as N-pyrrolic, result in more than 30-fold increase in the conductivity of semiconducting CNTs compared to Cu-incorporated CNTs alone. For metallic CNTs, the conductivity is in agreement with existing experimental data, and our prediction of significant increases in conductivity with N-pyrrolic functional group is consistent with recent experimental results, demonstrating the effectiveness of doping in modifying conductivity. In conclusion, our study provides valuable insight into the electronic properties of doped CNTs and contributes to the development of ultrahigh conductivity CNT composites.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Biexciton Condensation in Electron-Hole-Doped Hubbard Bilayers: A Sign-Problem-Free Quantum Monte Carlo Study

The bilayer Hubbard model with electron-hole doping is an ideal platform to study excitonic orders due to suppressed recombination via spatial separation of electrons and holes. However, suffering from the sign problem, previous quantum Monte Carlo studies could not arrive at an unequivocal conclusion regarding the presence of phases with clear signatures of excitonic condensation in bilayer Hubbard models. Here, we develop a determinant quantum Monte Carlo algorithm for the bilayer Hubbard model that is sign-problem-free for equal and opposite doping in the two layers and study excitonic order and charge and spin density modulations as a function of chemical potential difference between the two layers, on-site Coulomb repulsion, and interlayer interaction. In the intermediate coupling regime and in proximity to the SU(4)-symmetric point, we find a biexcitonic condensate phase at finite electron-hole doping, as well as a competing (π, π) charge density wave state. In this study, we extract the Berezinskii-Kosterlitz-Thouless transition temperature from superfluid density and a finite-size scaling analysis of the correlation functions and explain our results in terms of an effective biexcitonic hard-core boson model.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Modeling laser interactions with aluminum and tantalum targets using a hybrid atomistic-continuum model

A hybrid atomistic-continuum method can model the microstructure evolution of metals subjected to laser irradiation. This method combines classical molecular dynamics (MD) simulations with the two-temperature model (TTM) to account for the laser energy absorption and heat diffusion behavior. Accurate prediction of the temperature evolution in the combined MD-TTM method requires reliable accuracy in electron heat capacity, electron thermal conductivity, and electron–phonon coupling factor across the temperatures generated. This study uses the electronic density of states (DOS) obtained from first-principle calculations. The calculated electron temperature-dependent parameters are used in MD-TTM simulations to study the laser metal interactions in FCC and BCC metals and the phenomenon of laser shock loading and melting. This study uses FCC Al and BCC Ta as model systems to demonstrate this capability. When subjected to short pulsed laser shocks, the dynamic failure behavior predicted using temperature-dependent parameters is compared with the experimentally reported single-crystal and nanocrystalline Al and Ta systems. The MD-TTM simulations also investigate laser ablation and melting behavior of Ta to compare with the ablation threshold reported experimentally. In conclusion, this manuscript demonstrates that integrating the temperature-dependent parameters into MD-TTM simulations leads to the accurate modeling of the laser–metal interaction and allows the prediction of the kinetics of the solid–liquid interface.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Suppression of antiferromagnetic order and strong ferromagnetic spin fluctuations in Ca(Co 1-x Ni x ) 2-y As 2 single crystals

CaCo 2–y As 2 is a unique itinerant system having strong magnetic frustration. Here, we report the effect of electron doping on the physical properties resulting from Ni substitutions for Co. The single crystals of Ca(Co 1–x Ni x ) 2–y As 2 were characterized by single-crystal x-ray diffraction, energy-dispersive x-ray spectroscopy, magnetization M versus temperature T, magnetic field H, time t, and heat capacity C p (H, T) measurements. The A-type antiferromagnetic (AFM) transition temperature T N = 52 K for x = 0 decreases to 22 K with only 3% Ni substitution and is completely suppressed for x > 0.16. For 0.11 ≤ x ≤ 0.52 strong ferromagnetic (FM) fluctuations develop as revealed by magnetic susceptibility χ(T) = M(T) / H measurements. For x = 0.11 and 0.16 competing AFM and FM interactions result in a reentrant spin-glass behavior below T N , as evidenced by the observations of thermomagnetic hysteresis and magnetic relaxation. Enhanced FM fluctuations are also found for the x = 0.21 and 0.31 crystals, where χ c increases significantly at low T. A large χ anisotropy in these compositions where χ c is up to a factor of two larger than χ ab suggests that the FM spin fluctuations are quasi-1D in nature. Weak ferromagnetic contributions to the magnetization are found at T = 2 K for x = 0.11 –0.31. Heat-capacity Cp(T) measurements reveal the presence of FM quantum spin fluctuations for 0.11 ≤ x ≤ 0.52, where a logarithmic T dependence of Cp(T) / T is observed at low T. Here, the suppression of AFM order by the development of strong FM fluctuations in Ca(Co 1–x Ni x ) 2–y As 2 crystals suggests the presence of a FM quantum-critical point at x ≈ 0.20. Our density-functional theory (DFT) calculations confirm that FM fluctuations are enhanced by Ni substitutions for Co in CaCo 2–y As 2 . The Sommerfeld electronic heat-capacity coefficient is enhanced for x = 0, 0.21, and 0.42 by about a factor of two compared to DFT calculations of the density of states (DOS) at the Fermi energy, suggesting an enhancement of the DOS from electron-phonon and/or electron-electron interactions. The crystals with x > 0.52 do not exhibit FM spin fluctuations or magnetic order at T ≥ 1.8 K, which was found from the DFT calculations to arise from a Stoner transition. Superconductivity is not observed above 1.8 K for any of the compositions. Neutron-diffraction studies of crystals with x = 0.11 and 0.16 in the crossover regime (0.1 ≲ x ≲ 0.2) show no evidence of A-type ordering as observed in the parent compound with x = 0. Furthermore, no other common magnetic structures, such as ferromagnetic (FM), helical stacking of in-plane FM layers, or in-plane AFM structure, are found with an ordered moment greater than the uncertainty of 0.05 μ B per transition-metal atom.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Evolution of the electronic structure in Ta 2 NiSe 5 across the structural transition revealed by resonant inelastic x-ray scattering

We utilized high-energy-resolution resonant inelastic X-ray scattering (RIXS) at both the Ta and Ni L 3 -edges to map out element-specific particle-hole excitations in Ta 2 NiSe 5 across the phase transition. Our results reveal a momentum dependent gap-like feature in the low energy spectrum, which agrees well with the band gap in element-specific joint density of states calculations based on ab initio estimates of the electronic structure in both the low temperature monoclinic and the high temperature orthorhombic structure. Below T c , the RIXS energy-momentum map shows a minimal gap at the Brillouin zone center (~0.16 eV), conforming that Ta 2 NiSe 5 possesses a direct band gap in its low temperature ground state. However, inside the gap, no signature of anticipated collective modes with an energy scale comparable to the gap size can be identified. Upon increasing the temperature to above T c , whereas the gap at the zone center closes, the RIXS map at finite momenta still possesses the gross features of the low temperature map, suggesting a substantial mixing between the Ta and Ni orbits in the conduction and valence bands, which does not change substantially across the phase transition. Our experimental observations and comparison to the theoretical calculations lend further support that the phase transition and the corresponding gap opening in Ta 2 NiSe 5 is largely structural by nature with possible minor contribution from the putative exciton condensate.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

First-Principles Treatment of Vibrational Broadening in X-Ray Excited Valence Band Spectra for n-SrTiO 3 (001)

The valence band maximum (VBM) is an important quantity for semiconductors as it locates the Fermi level relative to the band edge. Accurate measurement of this quantity in near-surface regions of semiconductors by photoemission is a first step toward determining the electronic properties of heterostructures involving these materials. While extrapolating the leading edge of the valence band to the energy axis in photoemission spectra is a widely used way to find the VBM, this method can be ambiguous if the leading edge exhibits multiple slopes. Another way to determine the VBM is to fit the leading edge to an appropriately broadened, cross-section modulated theoretical density of states (DOS). Three kinds of broadening that should be included for maximum accuracy are those due to: (1) finite instrumental resolution, (2) valence hole lifetime, and (3) vibrational excitations. While steps (1) and (2) are straightforward to implement, (3) is more difficult because the appropriate amount of broadening is not known a priori. Here, we demonstrate that explicit inclusion of vibrational broadening using ab initio molecular dynamics facilitates accurate VBM determination for n-SrTiO 3 (001). The total DOS is constructed by summing time-averaged projections at elevated temperature onto s - , p - , and d orbitals for the constituent atoms and modulating with the associated photoemission cross sections. Subsequent convolutions of the total DOS, first with a Gaussian of width equal to the experimental energy resolution and second with a Lorentzian to simulate valence hole lifetime effects, yield line shapes that reproduce the experimental leading edges rather well. The VBM is then given by the energy at which the vibrationally broadened total DOS (prior to the convolutions) goes to zero. The VBMs generated by this method quantitatively agree with those resulting from extrapolating from the middle of the measured leading edge for SrTiO 3 .

36 MATERIALS SCIENCE↗