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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 865 records · Page 48
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Magnetization distribution in Cu 0.6 Mn 2.4 Ge 2 ferromagnet from polarized and non-polarized neutron powder diffraction aided by density-functional theory calculations

The crystal structure and magnetic properties of Cu 0.6 Mn 2.4 Ge 2 have been re-investigated by a combination of extensive magnetic measurements and neutron scattering experiments, aided by electronic structure calculations. The material is found to be a soft ferromagnet with the ordering temperature T C = 316 K. The magnetocaloric effect evaluated from field-dependent magnetization isotherms is equal to 1.2 J/(kg·K) and 2.5 J/(kg·K) under the maximum applied magnetic field of 2 T and 5 T, respectively. The compound crystallizes in the hexagonal space group P6 3 /mmc. A complex structural disorder necessitated testing of several disorder models against the results of non-polarized and polarized neutron scattering experiments and magnetization measurements. Simulations at the density-functional theory level were also performed to identify the most robust solution that properly described the data observed. The final magnetic structure model reveals non-equal magnetic moments on the Mn1 and Mn2 atoms (2.29(9) µ B and 2.7(1) µ B , respectively) and the presence of vacancies and minor Cu substitution defects in both Mn sites. The work demonstrates how the non-polarized and polarized neutron scattering methods can be combined with electronic structure calculations to establish the microscopic structure of magnetic materials with complex crystallographic disorder.

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

Quantum Composites with Charge-Density-Wave Fillers

Here, a unique class of advanced materials—quantum composites based on polymers with fillers composed of a van der Waals quantum material that reveals multiple charge-density-wave quantum condensate phases—is demonstrated. Materials that exhibit quantum phenomena are typically crystalline, pure, and have few defects because disorder destroys the coherence of the electrons and phonons, leading to collapse of the quantum states. The macroscopic charge-density-wave phases of filler particles after multiple composite processing steps are successfully preserved in this work. The prepared composites display strong charge-density-wave phenomena even above room temperature. The dielectric constant experiences more than two orders of magnitude enhancement while the material maintains its electrically insulating properties, opening a venue for advanced applications in energy storage and electronics. The results present a conceptually different approach for engineering the properties of materials, extending the application domain for van der Waals materials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Multilevel atomic structural model for interstratified opal materials

The structure of opal has long fascinated scientists. It occurs in a number of structural states, ranging from amorphous to exhibiting features of stacking disorder. Opal-CT, where C and T signify cristobalite- and tridymite-like interstratification, represents an important link in the length scales between amorphous and crystalline states. However, details about local atomic (dis)order and arrangements extending to long-range stacking faults in opal polymorphs remain incompletely understood. Here, a multilevel modeling approach is reported that considers stacking states in correlation with the abundance of C and T segments as a high-level structural parameter (i.e. not each atom). Optimization accounting for inter-tetrahedral bond lengths and angles and the regularity of the silicate tetrahedra is included as lower levels of structural parameters. Together, a set of parameters with both coarse-grained and atomistic features for different levels of structural details is refined. Structural disorder at the ~10–100 Å distance scale is evaluated using experimental pair distribution function and diffraction datasets, comparing peak intensities, widths and asymmetry. Here this work presents a complete multilevel structural description of natural opal-CT and explains many of the unusual features observed in X-ray powder diffraction patterns. This modeling approach can be adopted generally for analyzing layered materials and their assembly into 3D structures.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Reversibility and criticality in amorphous solids

The physical processes governing the onset of yield, where a material changes its shape permanently under external deformation, are not yet understood for amorphous solids that are intrinsically disordered. Here, using molecular dynamics simulations and mean-field theory, we show that at a critical strain amplitude the sizes of clusters of atoms undergoing cooperative rearrangements of displacements (avalanches) diverges. We compare this non-equilibrium critical behaviour to the prevailing concept of a ‘front depinning’ transition that has been used to describe steady-state avalanche behaviour in different materials. We explain why a depinning-like process can result in a transition from periodic to chaotic behaviour and why chaotic motion is not possible in pinned systems. As a result, these findings suggest that, at least for highly jammed amorphous systems, the irreversibility transition may be a side effect of depinning that occurs in systems where the disorder is not quenched.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Layered polymorph of titanium triiodide

A previously unreported layered spin ½ triangular lattice polymorph of TiI 3 is described, synthesized under 6 GPa of applied pressure at 900 °C, but stable at atmospheric pressure. This air-sensitive material has a CdI 2 -type layered structure (P-3m1 (no. 164), a = 4.012 Å and c = 6.641 Å at 120 K, Z = 1 of Ti 0.667 I 2 ) with an in-plane triangular lattice, related to that of TiI 4 (Ti 0.5 I 2 ). Although the TiI 3 formula is consistent with expectations for a layered honeycomb lattice of spin ½ Ti(III), there appears to be disorder in the crystal structure. Magnetic susceptibility and heat capacity measurements suggest that the material undergoes several low temperature phase transitions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Success and breakdown of the T-matrix approximation for phonon-disorder scattering

Here, we examine the validity of the widely used T-matrix approximation for treating phonon-disorder scattering by implementing an unfolding algorithm that allows simulation of disorder up to tens of millions of atoms. The T-matrix approximation breaks down for low-energy flexure phonons that play an important role in thermal transport in two-dimensional materials. Furthermore, insights are developed into the success of the T-matrix approximation in describing maximally mass disordered systems. To achieve this, the phonon unfolding formalism is generalized to describe mass disorder and strongly nonperturbative features of the spectrum are connected to the Boltzmann quasiparticle picture.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Thermodynamic controls on the synthesis, structure and reactivity of materials for energy (Final Report)

The major objectives have been: a) to advance and use unique calorimetric capabilities to determine the energetics of oxide and other materials having possible energy applications, with an emphasis on new materials for batteries, fuel cells and solar energy conversion, b) to understand, in terms of both macroscopic energetics and microscopic structure and bonding, the interplay of defect chemistry, oxidation-reduction, and size effects at the bulk and nanoscale in determining materials properties. This project emphasizes mixed ionic-electronic conduction materials containing transition metals of variable valence, especially perovskites and lithium containing phases, with M = Mn, Fe, Co, Ni. The thermochemistry of new families of complex halide, chalcogenide, nitride and hybrid (organic-inorganic) perovskite materials were explored. The major and unique technique employed is high temperature oxide melt solution calorimetry, with careful attention given to materials synthesis and characterization. The thermochemical studies will be coupled with structural studies, especially to characterize order-disorder phenomena by in situ high temperature diffraction techniques.

14 SOLAR ENERGY↗
DOE OSTI2023

Mechanical properties of an Al 10 Nb 20 Ta 15 Ti 30 V 5 Zr 20 A2/B2 refractory superalloy and its constituent phases

Refractory superalloys (RSAs) are a new class of high-temperature structural materials consisting of a nanometer-sized mixture of two coherent A2 (disordered BCC) and B2 (ordered) phases. While these RSAs typically exhibit superior mechanical properties at elevated temperatures, they suffer from limited plasticity at lower temperatures, often attributed to the continuous ordered B2 matrix in these two-phase alloys. To knowledgably control the microstructure and mechanical properties of these alloys, the properties of the constitutive phases in RSAs should be known. Currently this information is absent. Here, in the present work, the microstructure and mechanical properties (at 20–1200 °C) of a candidate Al 0.5 NbTa 0.8 Ti 1.5 V 0.2 Zr RSA and two single-phase alloys, which compositions correspond to the compositions of the A2 and B2 phases in the selected RSA, are reported. Interestingly, and quite unexpectedly, the intrinsic mechanical behavior of the constituent A2 and B2 phases, deciphered for the first time in the present study, revealed that they are softer and substantially more ductile than the parent two-phase RSA. Furthermore, the ordered B2 phase exhibits a deformation twinning mechanism leading to twinning induced plasticity (TWIP) coupled with a low APB energy and activity of 1/2<111> dislocations. These mechanisms are thought to be responsible for the high plasticity of the ordered B2 phase. The results presented here question the current assumption that the ordered B2 phase in these RSAs has limited plasticity and strongly indicate that the nature of the B2/A2 interface boundaries and coherency strengthening play an important role in controlling the mechanical properties of the two-phase RSA.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Robustness of Optical Response for Self-Assembled Plasmonic Metamaterials with Morphological Disorder and Surface Roughness

Bottom-up fabrication of metallized biotemplated nanostructures to form specific plasmonic nanoresonators holds promise as a means of achieving large-scale optical metamaterials. However, in contrast to top-down methods, the stochastic growth of self-assembled nanoresonators is prone to significant disorder and surface roughness, which naturally raise an important question about the robustness of their resonant properties in terms of structural imperfections. An aggregated-random-sphere model is developed to mimic the nucleated growth of metallized DNA origami assembly, leading to meta-atoms with realistic, experimentally observed morphological disorder and surface roughness. Using the well-known split-ring-resonator (SRR) motif as an example, the resonant properties of meta-atoms under different levels of roughness are investigated and a strong tolerance of optical response against morphological disorder is revealed. It is found that in SRRs, even with dramatic roughness introduced, the expected resonances are still observed, despite broadening line shapes compared to ideal smooth structure. Only for extreme disorder, which causes drastic segmentation of SRRs, does the resonant response disappear. Finally, the demonstrations are very encouraging for the prospects of bottom-up fabrication toward versatile functional metamaterials and metadevices.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Controlling Metastable Native Point-Defect Populations in Cu(In,Ga)Se 2 and Cu 2 ZnSnSe 4 Materials and Solar Cells through Voltage-Bias Annealing

Our contribution describes the influence of low-temperature annealing with and without applied voltage bias on thin-film Cu 2 ZnSnSe 4 (CZTSe), Cu(In,Ga)Se 2 (CIGS), and CdS material properties and solar cell performance. In order to quantify the effects of cation disorder on CZTSe device performance, completed devices were annealed under open-circuit conditions at various temperatures from 110 degrees C to 215 degrees C and subsequently quenched. Measurements on these devices document systematic, reversible changes in solar-cell performance consistent with a reduction in CZTSe band tails at lower annealing temperatures. CIGS and CZTSe solar cells were also annealed at various temperatures (200 degrees C for CIGS and 110 degrees C-215 degrees C for CZTSe) and subsequently quenched with continuously applied voltage bias to explore the effects of non-equilibrium annealing conditions. For both absorbers, large reversible changes in device characteristics correlated with the magnitude and sign of the applied voltage bias were observed. For CZTSe devices, the voltage-bias annealing (VBA) produced reversible changes in open-circuit voltage (VOC) from 289 meV to 446 meV. For CIGS solar cells, even larger changes were observed in device performance: photovoltaic (PV) conversion efficiency of the CIGS device varied from below 3% to above 15%, with corresponding changes in CIGS hole density of about three orders of magnitude. Findings from these VBA experiments are interpreted in terms of changes to the metastable point-defect populations that control key properties in the absorber layers, and in the CdS buffer layer. Computational device modeling was performed to assess the impacts of cation disorder on the CZTSe VOC deficit, and to elucidate the effects of VBA treatments on metastable point defect populations in CZTSe, CIGS, and CdS. Our results indicate that band tails impose important limitations on CZTSe device performance. Device modeling results also indicate that non-equilibrium processing conditions including the effects of voltage bias can dramatically alter point-defect-mediated opto-electronic properties of semiconductors. Implications for optimization of PV materials and connections to long-term stability of PV devices are discussed.

14 SOLAR ENERGY↗
DOE OSTI2017

Irradiation-induced defect formation and damage accumulation in single crystal CeO 2

Here, the accumulation of irradiation-induced disorder in single crystal CeO 2 has been investigated over a wide range of ion fluences. Room temperature irradiations of epitaxial CeO 2 thin films using 2 MeV Au 2+ ions were carried out up to a total fluence of 1.3 x 10 16 cm –2 Post-irradiation disorder was characterized using ion channeling Rutherford backscattering spectrometry (RBS/C) and confocal Raman spectroscopy. The Raman measurements were interpreted by means of a phonon confinement model, which employed rigid ion calculations to determine the phonon correlation length in the irradiated material. Comparison between the dose dependent changes in correlation length of the Raman measurements and the Ce disorder fraction from RBS/C provides complementary quantitative details on the rate of point and extended defect formation on the Ce and O sub-lattices over a broad range of ion fluences. Raman measurements, which are significantly more sensitive than RBS/C at low doses, reveal that the nucleation rate of defects is highest below 0.1 displacements per atom (dpa). Comparison between Raman and RBS/C measurements suggests that between 0.1 and 10 dpa the damage evolution is characterized by modest growth of point defects and/or small clusters, while above 10 dpa the preexisting defects rapidly grow into extended clusters and/or loops.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Effect of correlated oxide electrodes on disorder pinning and thermal roughening of ferroelectric domain walls in epitaxial PbZr 0.2 Ti 0.8 O 3 thin films

We report the competing effects of disorder pinning and thermal roughening on ferroelectric domain walls as a function of temperature in epitaxial PbZr 0.2 Ti 0.8 O 3 thin films deposited on (001) SrTiO 3 substrates buffered by three types of correlated oxide electrodes, La 0.67 Sr 0.33 MnO 3 , LaNiO 3 , and SrIrO 3 . Piezo-response force microscopy studies show that the 50 nm PbZr 0.2 Ti 0.8 O 3 films are uniformly polarized in the as-grown states, with the patterned domain structures persisting above 700 °C. For all three types of films, the domain wall roughness is dominated by 2D random bond disorder at room temperature, and transitions to 1D thermal roughening upon heating. The roughness exponent ζ increases progressively from 0.3 to 0.5 within a temperature window that depends on the bottom conducting oxide type, from which we extracted the distribution of disorder pinning energy. Lastly, we discuss the possible origins of the disorder pinning and the effect of the correlated oxide electrodes on the energy landscape of DW motion.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Insight into cation disorder of Li{sub 2}Fe{sub 0.5}Mn{sub 0.5}SiO{sub 4}

Transition metal lithium orthosilicates are promising cathode materials for lithium-ion batteries. Here we report a combined experimental (in situ X-ray diffraction) and computational (static lattice and molecular dynamics) study of the thermal behavior of the Li{sub 2}Fe{sub 0.5}Mn{sub 0.5}SiO{sub 4} orthosilicate from room temperature to 950 °C. Our X-ray results showed that Pmnb polymorph is the most stable all over the explored temperature range. A significant cation disorder up to 80%, based on the anti-site defect, was found. The defect concentration depends on the synthesis route and temperature, and is completely reversible after the thermal treatments. Moreover, a careful analysis of the impurity phases allowed us to identify Li{sub 2}SiO{sub 3}, Fe{sub 3}O{sub 4} and Li{sub 3}Fe{sub 5}O{sub 8}, the last one never reported before. The minimization of defects by opportunely tuning the synthetic parameters would be of great importance in view of potential applications of these materials in lithium batteries. - Graphical abstract: A combined experimental in situ X-ray diffraction and computational study of the thermal behavior of the Li{sub 2}Fe{sub 0.5}Mn{sub 0.5}SiO{sub 4} is reported herein. The anti-site defect does justify the diffraction patterns changes with temperature. Highlights: ► Study of the thermal behavior of Li{sub 2}Fe{sub 0.5}Mn{sub 0.5}SiO{sub 4}. ► The anti-site defect does justify the diffraction patterns changes with temperature. ► The Pmnb polymorph is stable in the investigated temperaturerange.

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

Erbium-implanted materials for quantum communication applications

Erbium-doped materials can serve as spin-photon interfaces with optical transitions in the telecom C band, making them an exciting class of materials for long-distance quantum communication. However, the spin and optical coherence times of Er 3+ ions are limited by currently available host materials, motivating the development of new Er 3+ -containing materials. Here we demonstrate the use of ion implantation to efficiently screen prospective host candidates, and show that disorder introduced by ion implantation can be mitigated through post-implantation thermal processing to achieve inhomogeneous linewidths comparable to bulk linewidths in as-grown samples. We present optical spectroscopy data for each host material, which allows us to determine the level structure of each site, allowing us to compare the environments of Er 3+ introduced via implantation and via doping during growth. Here, we demonstrate that implantation can generate a range of local environments for Er 3+ , including those observed in bulk-doped materials, and that the populations of these sites can be controlled with thermal processing.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Progress towards subsurface spectroscopy inside heterogeneous materials using four wave mixing phase conjugation

Herein, we report preliminary results on subsurface spectroscopy inside heterogeneous materials using four wave mixing phase conjugation. For our test material we use an inert plastic bonded explosive simulant that contains fluorescent guidestar particles. Using phase conjugation, we are able to obtain spectral enhancements approximately equal to the phase conjugate reflectivity. Additionally, we discuss future directions to improve this technique to obtain greater signal enhancements.

47 OTHER INSTRUMENTATION↗
NASA NTRS1978

X-ray diffractometer studies of shocked materials

This study explores the utility of X-ray diffractometer scans for determination of shock pressure histories of geological materials from meteorite impact sites. The technique is based on quantification of increased crystal lattice disorder with increasing shock pressure as expressed by decreasing diffraction peak amplitude and pronounced line-broadening caused by decreasing mosaic domain size and increasing strain. The ratio of peak height (PH) to half width (HW) decreases systematically with increasing shock pressure. Data are given for experimentally shocked quartz, feldspars, pyroxene and olivine along with data for granitic materials from the Piledriver nuclear event and from the Ries Crater, Germany. Although the technique in principle may be capable of yielding relatively accurate pressure determinations, its application to naturally shocked materials may be severely limited.

Hanss, R. E.↗
DOE OSTI2023

Systematic modification of functionality in disordered elastic networks through free energy surface tailoring

A combined machine learning–physics–based approach is explored for molecular and materials engineering. Specifically, collective variables, akin to those used in enhanced sampled simulations, are constructed using a machine learning model trained on data gathered from a single system. Through the constructed collective variables, it becomes possible to identify critical molecular interactions in the considered system, the modulation of which enables a systematic tailoring of the system’s free energy landscape. To explore the efficacy of the proposed approach, we use it to engineer allosteric regulation and uniaxial strain fluctuations in a complex disordered elastic network. Its successful application in these two cases provides insights regarding how functionality is governed in systems characterized by extensive connectivity and points to its potential for design of complex molecular systems.

42 ENGINEERING↗