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Results for “Crystal field theory”

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 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
NASA NTRS2005

Stability of Magnetically-Suppressed Solutal Convection In Protein Crystal Growth

The effect of convection during the crystallization of proteins is not very well understood. In a gravitational field, convection is caused by crystal sedimentation and by solutal buoyancy induced flow and these can lead to crystal imperfections. While crystallization in microgravity can approach diffusion limited growth conditions (no convection), terrestrially strong magnetic fields can be used to control fluid flow and sedimentation effects. In this work, a theory is presented on the stability of solutal convection of a magnetized fluid in the presence of a magnetic field. The requirements for stability are developed and compared to experiments performed within the bore of a superconducting magnet. The theoretical predictions are in good agreement with the experiments and show solutal convection can be stabilized if the surrounding fluid has larger magnetic susceptibility and the magnetic field has a specific structure. Discussion on the application of the technique to protein crystallization is also provided.

Leslie, F. W.↗
NASA NTRS2006

Using Magnetic Field Gradients to Simulate Variable Gravity in Fluids and Materials Experiments

Fluid flow due to a gravitational field is caused by sedimentation, thermal buoyancy, or solutal buoyancy induced convection. During crystal growth, for example, these flows are undesirable and can lead to crystal imperfections. While crystallization in microgravity can approach diffusion limited growth conditions (no convection), terrestrially strong magnetic fields can be used to control fluid flow and sedimentation effects. In this work, a theory is presented on the stability of solutal convection of a magnetized fluid(weak1y paramagnetic) in the presence of a magnetic field. The requirements for stability are developed and compared to experiments performed within the bore of a superconducting magnet. The theoretical predictions are in good agreement with the experiments. Extension of the technique can also be applied to study artificial gravity requirements for long duration exploration missions. Discussion of this application with preliminary experiments and application of the technique to crystal growth will be provided.

Ramachandran, Narayanan↗
DOE OSTI2023

Role of spin-orbit coupling on crystal-field splitting and phase-stability of rare-earth based layered intermetallic

Layered and incommensurate heterostructures have attracted much attention for the occurrence of superconductivity and charge density waves with the possibility of intercalating foreign atoms. However, lanthanide-based heterostructures where (Eu x Sm 1-x )S and TaS 2 are alternatively stacked have been scarcely investigated. In this work, we performed phase stability, bonding behavior and electronic-structure analysis of (Eu x Sm 1-x )TaS 3 using first-principles density-functional theory methods. Our phase stability analysis suggests 50 at.% solubility of Eu in (Eu x Sm 1-x )TaS 3 compared to Eu solubility in all proportions in cubic SmS. The instability of Eu beyond 50 at.% in (Eu x Sm 1-x )TaS 3 was attributed to higher density of Eu-4f states at the Fermi-level. Based on band position calculated from spin-orbit coupling effect, we constructed a qualitative schematic of possible crystal-field analysis. The local change in bond-length and bond-angle around Eu-S in (Eu x Sm 1-x )TaS 3 correlate well with our crystal-field analysis. We believe that quantum mechanical insights provided in this work will be useful to understand other complex heterostructures.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Fermi surfaces of the topological semimetal CaSn 3 probed through de Haas van Alphen oscillations

Abstract In the search of topological superconductors, nailing down the Fermiology of the normal state is as crucial a prerequisite as unraveling the superconducting pairing symmetry. In particular, the number of time-reversal-invariant momenta (TRIM) in the Brillouin zone enclosed by Fermi surfaces is closely linked to the topological class of time-reversal-invariant systems, and can experimentally be investigated. We report here a detailed study of de Haas van Alphen quantum oscillations in single crystals of the topological semimetal CaSn 3 with torque magnetometry in high magnetic fields up to 35 T. In conjunction with density functional theory based calculations, the observed quantum oscillations frequencies indicate that the Fermi surfaces of CaSn 3 enclose an odd number of TRIM, satisfying one of the proposed criteria to realize topological superconductivity. Nonzero Berry phases extracted from the magnetic oscillations also support the nontrivial topological nature of CaSn 3 .

Physics↗
NASA NTRS1982

Direct observation of interface instability during crystal growth

The general aim of this investigation was to study interface stability and solute segregation phenomena during crystallization of a model system. Emphasis was to be placed on direct observational studies partly because this offered the possibility at a later stage of performing related experiments under substantially convection-free conditions in the space shuttle. The major achievements described in this report are: (1) the development of a new model system for fundamental studies of crystal growth from the melt and the measurement of a range of material parameters necessary for comparison of experiment with theory. (2) The introduction of a new method of measuring segregation coefficient using absorption of a laser beam by the liquid phase. (3) The comparison of segregation in crystals grown by gradient freezing and by pulling from the melt. (4) The introduction into the theory of solute segregation of an interface field term and comparison with experiment. (5) The introduction of the interface field term into the theories of constitutional supercooling and morphological stability and assessment of its importance.

Tiller, W. A.↗
NASA NTRS1972

Effect of a magnetic field on the diffusion of an electron-hole plasma in germanium.

Study in germanium of an optically injected electron-hole plasma, parallel and perpendicular to an applied magnetic field. The density gradient within the crystal was measured directly by an infrared-beam-absorption technique. Diffusion measurements made parallel to the magnetic field are adequately explained by the theory.

Gurnee, M. N.↗
NASA NTRS1988

Electronic materials high-T(sub c) superconductivity polymers and composites structural materials surface science and catalysts industry participation

The fifth year of the Center for Advanced Materials was marked primarily by the significant scientific accomplishments of the research programs. The Electronics Materials program continued its work on the growth and characterization of gallium arsenide crystals, and the development of theories to understand the nature and distribution of defects in the crystals. The High Tc Superconductivity Program continued to make significant contributions to the field in theoretical and experimental work on both bulk materials and thin films and devices. The Ceramic Processing group developed a new technique for cladding YBCO superconductors for high current applications in work with the Electric Power Research Institute. The Polymers and Composites program published a number of important studies involving atomistic simulations of polymer surfaces with excellent correlations to experimental results. The new Enzymatic Synthesis of Materials project produced its first fluorinated polymers and successfully began engineering enzymes designed for materials synthesis. The structural Materials Program continued work on novel alloys, development of processing methods for advanced ceramics, and characterization of mechanical properties of these materials, including the newly documented characterization of cyclic fatigue crack propagation behavior in toughened ceramics. Finally, the Surface Science and Catalysis program made significant contributions to the understanding of microporous catalysts and the nature of surface structures and interface compounds.

Source record↗
DOE OSTI2025

Interface morphology and dislocation-mediated processes during rapid solidification of thin films

Rapid solidification experiments have, in recent years, revealed a wealth of new microstructural phenomena that suggest a strong connection between the kinetics of solidification and the crystalline structures that emerge as a result. In this work, we investigate the interplay between interface morphology and defect-mediated processes during rapid solidification conditions using a Phase Field Crystal (PFC) model, enabling us to simultaneously and efficiently explore the physics of solidification and elasto-plasticity in the formalism of a single-field theory. We predict that there are two mechanisms by which dislocations emitted directly from the solid–liquid interface induce orientation gradients as well as the formation of subgrain boundaries within a single solidifying cell. We relate these mechanisms to the morphology of the moving solid–liquid interface and identify a suitable control parameter in the PFC model with which we can go between said morphologies by effectively changing the relative strength of the capillary length and kinetic coefficients of the solid–liquid interface. Thus, we are able to provide mechanistic explanations for several microstructural features (with an emphasis on orientation gradients and subgrain boundaries) observed during the rapid solidification of pure materials. We also provide a simple explanation for the formation of “jagged” subgrain boundaries, which is consistent with our experimental observations in rapidly solidified samples of Aluminum, whose mechanisms have thus far been unknown.

Interface morphology↗
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

Scaling laws for two-dimensional dendritic crystal growth in a narrow channel

Here, we investigate analytically and computationally the dynamics of two-dimensional needle crystal growth from the melt in a narrow channel. Our analytical theory predicts that, in the low supersaturation limit, the growth velocity $\textit{V}$ decreases in time $\textit{t}$ as a power law $V ~t^{–2/3}$, which we validate by phase-field and dendritic-needle-network simulations. Simulations further reveal that, above a critical channel width $Λ ≈ 5l_D$, where $l_D$ is the diffusion length, needle crystals grow with a constant $V < V_s$, where $V_s$ is the free-growth needle crystal velocity, and approaches $V_s$ in the limit $Λ \gg l_D$.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Fermi surface topology and magnetotransport properties of superconducting Pd 3 Bi 2 Se 2

Pd 3 Bi 2 Se 2 is a rare realization of a superconducting metal with a non-zero topological invariant. Here, in this study, we report the growth of high-quality single crystals of layered Pd 3 Bi 2 Se 2 with a superconducting transition at T c ≈ 0.80 K and upper critical fields of ~10 mT and ~5 mT for the in plane and out-of-plane directions, respectively. Our density functional theory (DFT) calculations reveal three pairs of doubly degenerate bands crossing the Fermi level all displaying clear three dimensional dispersion consistent with the overall low electronic anisotropy (<2). The multiband electronic nature of Pd 3 Bi 2 Se 2 is evident in magneto-transport measurements, yielding a sign changing Hall resistivity at low temperatures. The magnetoresistance is non-saturating and follows Kohler’s scaling rule. We interpret the magneto-transport data in terms of open orbits that are revealed in the DFT calculated Fermi surface. de Haas-van Alphen (dHvA) oscillation measurements using torque magnetometry on single crystals yield four frequencies for out-of-plane fields: F α = (150 ± 26) T, F β = (293 ± 10) T, F γ = (375 ± 20) T and F η = (1017 ± 12) T, with the low frequency dominating the spectrum. Through the measurement of angular dependent dHvA oscillations and DFT calculations we identify the F α frequency with an approximately ellipsoidal electron pocket centered on the L 2 point of the Brillouin zone. Lifshitz-Kosevich analysis of the dHvA oscillations reveals a small cyclotron effective mass m* = (0.11 ± 0.02)m 0 and a nontrivial Berry phase for the dominant orbit. The presence of nontrivial topology in a bulk superconductor positions Pd 3 Bi 2 Se 2 as a potential candidate for exploring topological superconductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

First-Principles Calculations of Thermoelectric Transport Properties of Quaternary and Ternary Bulk Chalcogenide Crystals

Chalcogenide crystals have a wide range of applications, especially as thermoelectric materials for energy conversion. Thermoelectric materials can be used to generate an electric current from a temperature gradient based on the Seebeck effect and based on the Peltier effect, and they can be used in cooling applications. Using first-principles calculations and semiclassical Boltzmann theory, we have computed the Seebeck coefficient, electrical conductivity, electronic thermal conductivity, power factor, and figure of merit of 30 chalcogenide crystals. A Quantum Espresso package is used to calculate the electronic properties and locate the Fermi level. The transport properties are then calculated using the BoltzTraP code. The 30 crystals are divided into two groups. The first group has four crystals with quaternary composition (A 2 BCQ 4 ) (A = Tl; B = Cd, Hg; C = Si, Ge, Sn; Q = S, Se, Te). The second group contains 26 crystals with the ternary composition (A’B’Q 2 ) (A’ = Ag, Cu, Au, Na; B’ = B, Al, Ga, In; Q = S, Se, Te). Among these 30 chalcogenide crystals, the results for 11 crystals: Tl 2 CdGeSe 4 , Tl 2 CdSnSe 4 , Tl 2 HgSiSe 4 , Tl 2 HgSnS 4 , AuBSe 2 , AuBTe 2 , AuAlTe 2 , AuGaTe 2 , AuInTe 2 , AgAlSe 2 , and AgAlTe 2 are revealed for the first time. In addition, temperature-dependent transport properties of pure and doped AgSbSe 2 and AgSbTe 2 crystals with dopant compositions of AgSb 0.94 Cd 0.06 Te 2 and AgSbTe 1.85 Se 0.15 were explored. These results provide an excellent database for bulk chalcogenides crucial for a wide range of potential applications in renewable energy fields.

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

Analytical Model for Atomic Relaxation in Twisted Moiré Materials

By virtue of being atomically thin, the electronic properties of heterostructures built from two-dimensional materials are strongly influenced by atomic relaxation. The atomic layers behave as flexible membranes rather than rigid crystals. Here we develop an analytical theory of lattice relaxation in twisted moiré materials. We obtain analytical results for the lattice displacements and corresponding pseudo gauge fields, as a function of twist angle. We benchmark our results for twisted bilayer graphene and twisted WSe 2 bilayers using large-scale molecular dynamics simulations. Our single-parameter theory is valid in graphene bilayers for twist angles 𝜃 ≳ 0.7°, and in twisted WSe 2 for 𝜃 ≳ 1.6°. Furthermore, we also investigate how relaxation alters the electronic structure in twisted bilayer graphene, providing a simple extension to the continuum model to account for lattice relaxation.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Backbone Stitching in Bottlebrush Copolymer Mesodomains and the Impact of Side Chain Crystallization

We synthesized bottlebrush statistical copolymers (BSCPs) having poly­(ethylene oxide) (PEO) and poly­(dimethylsiloxane) (PDMS) side chains attached to a polynorbornene backbone. Small-angle X-ray scattering analysis showed that for densely grafted BSCPs, the scattering length density gradually transitions between the PEO and PDMS domains. For loosely grafted BSCPs, the polymer backbone formed a distinct mesodomain, with a lower electron and mass density than both the PEO and PDMS domains. The bottlebrush backbone essentially “stitches” the PEO and PDMS side chains, looping back and forth from the PEO to PDMS domains with the backbone segments oriented normal to the domain interfaces. Self-consistent field theory (SCFT) calculations validated the stitching of the backbone driven by the microphase separation of PEO and PDMS, along with a strong segmental order of the side chains in the melt. The reduced birefringence upon PEO crystallization suggests the disruption of the strong segmental order by the crystallization. Both the static intrinsic and the form birefringences of the BSCPs decreased upon PEO crystallization. Solid-state NMR confirmed the rigidity of PEO crystallites and the bottlebrush backbone. Self-assembly of BSCPs containing polyhedral oligomeric silsesquioxane (POSS) pendent groups was also evaluated by X-ray scattering, showing the formation of lamellar microdomains that inhibited POSS crystallization.

Hu, Mingqiu↗
DOE OSTI2023

Revealing topology in metals using experimental protocols inspired by K-theory

Topological metals are conducting materials with gapless band structures and nontrivial edge-localized resonances. Their discovery has proven elusive because traditional topological classification methods require band gaps to define topological robustness. Inspired by recent theoretical developments that leverage techniques from the field of C*-algebras to identify topological metals, here, we directly observe topological phenomena in gapless acoustic crystals and realize a general experimental technique to demonstrate their topology. Specifically, we not only observe robust boundary-localized states in a topological acoustic metal, but also re-interpret a composite operator—mathematically derived from the K-theory of the problem—as a new Hamiltonian whose physical implementation allows us to directly observe a topological spectral flow and measure the topological invariants. Our observations and experimental protocols may offer insights for discovering topological behaviour across a wide array of artificial and natural materials that lack bulk band gaps.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Polycrystal thermo-elasticity revisited: theory and applications

The self-consistent (SC) theory is the most commonly used mean-field homogenization method to estimate the mechanical response behavior of polycrystals based on the knowledge of the properties and orientation distribution of constituent single-crystal grains. The original elastic SC method can be extended to thermo-elasticity by adding a stress-free strain to an elastic constitutive relation that expresses stress as a linear function of strain. With the addition of this independent term, the problem remains linear. Although the thermo-elastic self-consistent (TESC) model has important theoretical implications for the development of self-consistent homogenization of non-linear polycrystals, in this paper, we focus on TESC applications to actual thermo-elastic problems involving non-cubic (i.e. thermally anisotropic) materials. To achieve this aim, here we provide a thorough description of the TESC theory, which is followed by illustrative examples involving cooling of polycrystalline non-cubic metals. The TESC model allows studying the effect of crystallographic texture and single-crystal elastic and thermal anisotropy on the effective thermo-elastic response of the aggregate and on the internal stresses that develop at the local level.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Defect-driven ferrimagnetism and hidden magnetization in MnBi 2 Te 4

MnBi 2 Te 4 (MBT) materials are promising antiferromagnetic topological insulators in which field-driven ferromagnetism is predicted to cause a transition between axion insulator and Weyl semimetallic states. However, the presence of antiferromagnetic coupling between Mn/Bi antisite defects and the main Mn layer can reduce the low-field magnetization, and it has been shown that such defects are more prevalent in the structurally identical magnetic insulator MnSb 2 Te 4 (MST). We use high-field magnetization measurements to show that the magnetization of MBT and MST occur in stages and full saturation requires fields of ~60 T. As a consequence, the low-field magnetization plateau state in MBT, where many determinations of the quantum anomalous Hall state are studied, actually consists of ferrimagnetic septuple blocks containing both uniform and staggered magnetization components.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1973

The effect of surface conditions on the work function of insulators and semiconductors

Ionization energies of organic semiconductors were determined using single crystals of the material. The theory of the method is essentially that of Millikan's oil drop experiment. The technique employed in the experiment is based on the electrostatic method of balancing a charged particle in an electric field against the force of gravity for different excitation energies above the threshold value, and from an estimate of the balancing voltages, read off the ionization energy from the intercept of the energy axis in a plot wavelength corresponding to the balancing potential for the incident radiation of wavelength. In the modified technique which is adopted in the present experimental investigation, a small single crystal is suspended by a fine quartz fiber between two vertical capacitor plates to which a suitable high voltage is applied.

George, A.↗