Vacancy-suppressed lattice conductivity of high- ZT In 4 Se 3 - x
Explore the source record for details and available documents.
charge transport↗
SEARCH · Engineering Papers
Results for “point defect”
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.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
Multiple high-temperature transitions driven by dynamical structures in NaI
Abstract not provided
Manley, M. E.↗
Anharmonic properties in M g 2 X ( X = C , Si , Ge , Sn , Pb ) from first-principles calculations
Thermal conductivity reduction is one of the potential routes to improve the performance of thermoelectric materials. Yet, detailed understanding of the thermal transport of many promising materials is still missing. In this paper, we employ electronic-structure calculations at the level of density functional theory to elucidate thermal transport properties of the Mg 2 X (X = C , Si, Ge, Sn, and Pb) family of compounds, which includes M g 2 Si , a material already identified as a potential thermoelectric. All these materials crystallize into the same antifluorite structure. Systematic trends in the anharmonic properties of these materials are presented and examined. These calculations indicate that the reduction in the group velocity is the main driver of the thermal conductivity trend in these materials, as the phonon lifetimes in these compounds are very similar. We also examine the limits of the applicability of perturbation theory to study the effect of point defects on thermal transport and find that it is in good agreement with experiment in a wide range of scattering parameter values. The thermal conductivity of the recently synthesized Mg 2 C is computed and predicted to be 34 W/mK at 300°C.
36 MATERIALS SCIENCE↗
Electron-phonon coupling and thermal transport in the thermoelectric compound Mo 3 Sb 7–x Te x
Phonon properties of Mo 3 Sb 7–x Te x (x = 0, 1.5, 1.7), a potential high-temperature thermoelectric material, have been studied with inelastic neutron and x-ray scattering, and with first-principles simulations. The substitution of Te for Sb leads to pronounced changes in the electronic struc- ture, local bonding, phonon density of states (DOS), dispersions, and phonon lifetimes. Alloying with tellurium shifts the Fermi level upward, near the top of the valence band, resulting in a strong suppression of electron-phonon screening, and a large overall stiffening of interatomic force- constants. The suppression in electron-phonon coupling concomitantly increases group velocities and suppresses phonon scattering rates, surpassing the effects of alloy-disorder scattering, and re- sulting in a surprising increased lattice thermal conductivity in the alloy. We also identify that the local bonding environment changes non-uniformly around different atoms, leading to variable perturbation strengths for different optical phonon branches. The respective roles of changes in phonon group velocities and phonon lifetimes on the lattice thermal conductivity are quantified. Lastly, our results highlight the importance of the electron-phonon coupling on phonon mean-free-paths in this compound, and also estimates the contributions from boundary scattering, umklapp scattering, and point-defect scattering.
36 MATERIALS SCIENCE↗
Resonant optical spectroscopy and coherent control of C r 4 + spin ensembles in SiC and GaN
Spins bound to point defects are increasingly viewed as an important resource for solid-state implementations of quantum information technologies. In particular, there is a growing interest in the identification of new classes of defect spin that can be controlled optically. Here we demonstrate ensemble optical spin polarization and optically detected magnetic resonance (ODMR) of the S = 1 electronic ground state of chromium (Cr 4+ ) impurities in silicon carbide (SiC) and gallium nitride (GaN). Polarization is made possible by the narrow optical linewidths of these ensembles (< 8.5 GHz), which are similar in magnitude to the ground state zero-field spin splitting energies of the ions at liquid helium temperatures. We therefore are able to optically resolve individual spin sublevels within the ensembles at low magnetic fields using resonant excitation from a cavity-stabilized, narrow-linewidth laser. Additionally, these near-infrared emitters possess exceptionally weak phonon sidebands, ensuring that > 73% of the overall optical emission is contained with the defects’ zero-phonon lines. Lastly, these characteristics make this semiconductor-based, transition metal impurity system a promising target for further study in the ongoing effort to integrate optically active quantum states within common optoelectronic materials.
36 MATERIALS SCIENCE↗
Copper interstitial recombination centers in Cu 3 N
We present a comprehensive study of the earth-abundant semiconductor Cu 3 N as a potential solar energy conversion material, using density functional theory and experimental methods. Density functional theory indicates that among the dominant intrinsic point defects, copper vacancies V Cu have shallow defect levels while copper interstitials Cu i behave as deep potential wells in the conduction band which mediate Shockley-Read-Hall recombination. The existence of Cu i defects has been experimentally verified using photothermal deflection spectroscopy. A Cu 3 N/ZnS heterojunction diode with good current-voltage rectification behavior has been demonstrated experimentally, but no photocurrent is generated under illumination. Finally, the absence of photocurrent can be explained by a large concentration of Cu i recombination centers capturing electrons in p-type Cu 3 N.
14 SOLAR ENERGY↗
Neutron studies of gauge field and charge in Ih heavy-water ice
The distinctive character of water ice results from the partially disordered combination of covalent and hydrogen bonds in the network of hydrogen and oxygen atoms. The nontrivial hydrogen correlations we report in diffuse neutron scattering are analytically fit via a description of this state as a topological system exhibiting an emergent gauge field. This enables the density of correlation-terminating point defects to be decided as one defect per 500 oxygen sites at 30 K. Application of an analytical model of ice paves the way towards a detailed understanding of this ubiquitous solid.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Nematic-Field-Driven Positioning of Particles in Liquid Crystal Droplets
Common nematic oils, such as 5CB, experience planar anchoring at aqueous interfaces. When these oils are emulsified, this anchoring preference and the resulting topological constraints lead to the formation of droplets that exhibit one or two point defects within the nematic phase. Here, we explore the interactions of adsorbed particles at the aqueous interface through a combination of experiments and coarse-grained modeling, and demonstrate that surface-active particles, driven by elastic forces in the droplet, readily localize to these defect regions in a programmable manner. When droplets include two nanoparticles, these preferentially segregate to the two poles, thereby forming highly regular dipolar structures that could serve for hierarchical assembly of functional structures. Finally, addition of sufficient concentrations of surfactant changes the interior morphology of the droplet, but pins defects to the interface, resulting in aggregation of the two particles.
42 ENGINEERING↗
Breaking Rayleigh’s Law with Spatially Correlated Disorder to Control Phonon Transport
Controlling thermal transport in insulators and semiconductors is crucial for many technological fields such as thermoelectrics and thermal insulation, for which a low thermal conductivity (κ) is desirable. A major obstacle for realizing low κ materials is Rayleigh’s law, which implies that acoustic phonons, which carry most of the heat, are insensitive to scattering by point defects at low energy. We demonstrate, with large scale simulations on tens of millions of atoms, that isotropic long-range spatial correlations in the defect distribution can dramatically reduce phonon lifetimes of important low-frequency heat-carrying modes, leading to a large reduction of κ—potentially an order of magnitude at room temperature. We propose a general and quantitative framework for controlling thermal transport in complex functional materials through structural spatial correlations, and we establish the optimal functional form of spatial correlations that minimize κ. Finally, we end by briefly discussing experimental realizations of various correlated structures.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Strain annealing of SiC nanoparticles revealed through Bragg coherent diffraction imaging for quantum technologies
The crystalline strain properties of nanoparticles have broad implications in a number of emerging fields, including quantum and biological sensing in which heterogeneous internal strain fields are detrimental to performance. Here we used synchrotron-based Bragg coherent x-ray diffraction imaging (BCDI) to measure three-dimensional lattice strain fields within individual 3C-SiC nanoparticles, a candidate host material for quantum sensing, as a function of temperature during and after annealing up to 900 degrees C. We observed pronounced homogenization of the initial strain field at temperatures above 500 degrees C, and we find that the surface layers and central volumes of the nanoparticles reduce strain at similar rates, suggesting a uniform healing mechanism. Thus, we attribute the observed strain homogenization to activation of mobile point defects that annihilate and improve the overall quality of the crystal lattice. This work also establishes the feasibility of performing BCDI at high temperatures (up to 900 degrees C) to map structural hystereses relevant to the processing of quantum nanomaterials.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Emulating 2D Materials with Magnons
Spin waves (magnons) in two-dimensional (2D) materials have received increasing interest due to their unique states and potential for tunability. However, many interesting features of these systems, including Dirac points and topological states, occur at high frequencies, where experimental probes are limited. Here, we study a crystal formed by patterning a hexagonal array of holes in a perpendicularly magnetized thin film. Through simulation, we find that the magnonic band structure imitates that of graphene, but additionally has some kagomelike character and includes a few flat bands. Surprisingly, its nature can be understood using a nine-band tight-binding Hamiltonian. This clear analogy to 2D materials enables band-gap engineering in 2D, topological magnons along 1D phase boundaries, and spectrally isolated modes at 0D point defects. Interestingly, the 1D phase boundaries allow access to the valley degree of freedom through a magnonic analog of the quantum valley Hall insulator. These approaches can be extended to other magnonic systems, but are potentially more general due to the simplicity of the model, which resembles existing results from electron, phonon, photon, and cold-atom systems. This finding brings the physics of spin waves in 2D materials to more experimentally accessible scales, augments it, and outlines a few principles for controlling magnonic states.
Ferrimagnets↗
Weak localization and universal conductance fluctuations in large-area twisted bilayer graphene
We study diffusive magnetotransport in highly 𝑝-doped large-area twisted bilayer graphene in 1∘, 7∘, 9∘, and 20∘ samples. All samples exhibit weak localization, from which we extract the phase coherence length and intervalley scattering lengths, and from that determine that dephasing is caused by electron-electron scattering and intervalley scattering is caused by point defects. We observe signatures of universal conductance fluctuations in the 9∘ sample, which has high mobility and is near the van Hove singularity. Further improvements in sample quality and applications to large-area moiré materials will open new avenues to observe quantum interference effects.
Talkington, Spenser [University of Pennsylvania]↗
Debye–Waller coefficient of heavily deformed nanocrystalline iron
Synchrotron radiation X-ray diffraction (XRD) patterns from an extensively ball-milled iron alloy powder were collected at 100, 200 and 300 K. The results were analysed together with those using extended X-ray absorption fine structure, measured on the same sample at liquid nitrogen temperature (77 K) and at room temperature (300 K), to assess the contribution of static disorder to the Debye–Waller coefficient ( B iso ). Both techniques give an increase of ~20% with respect to bulk reference iron, a noticeably smaller difference than reported by most of the literature for similar systems. Besides good quality XRD patterns, proper consideration of the temperature diffuse scattering seems to be the key to accurate values of the Debye–Waller coefficient. Molecular dynamics simulations of nanocrystalline iron aggregates, mapped on the evidence provided by XRD in terms of domain size distribution, shed light on the origin of the observed B iso increase. The main contribution to the static disorder is given by the grain boundary, while line and point defects have a much smaller effect.
36 MATERIALS SCIENCE↗
Intermixing and Formation of Cu-Rich Secondary Phases at Sputtered CdS/CuInGaSe 2 Heterojunctions
In this work, the Cu migration behavior in PVD-CdS/PVD-Cu(In,Ga)Se 2 (CIGS) heterojunctions is investigated by high-resolution electron microscopy (HREM) and energy dispersive X-ray spectroscopy (EDS). Incorporation of Cu into the CdS forms Cu-rich domains but has no effect on epitaxy of the CdS. Epitaxy is commonly observed in the CdS studied. Secondary ion mass spectroscopy depth profiles confirm the presence of Cu in the CdS. In some cases, Cd is completely replaced by Cu, resulting in a Cu-S binary compound epitaxially grown on the CIGS and fully coherent with the surrounding CdS. This is most likely to be cubic Cu 2 S, based on lattice spacing measurements from HREM images and EDS elemental quantification. In addition, we find that the buffer layer crystal structure influences the extent of Ga depletion at the CIGS surface, which is more pronounced adjacent to zinc-blende CdS than wurtzite CdS. Density functional theory calculations reveal that Cu clustering and different Ga depletion widths can be attributed to the inherent anisotropy of wurtzite CdS and differences in CIGS point-defect migration barriers. Understanding the influence of these effects on device properties is a critical step in developing more efficient CdS/CIGS-based photovoltaics.
14 SOLAR ENERGY↗
Moving Beyond p-Type mc-Si: Quantified Measurements of Iron Content and Lifetime of Iron-Rich Precipitates in n-Type Silicon
N-type multicrystalline silicon (mc-Si) is a promising alternative to the dominant p-type mc-Si for solar cells because it combines the cost advantages of mc-Si while benefiting from higher tolerance to transition metal contamination. A detailed understanding of the relative roles of point defect and precipitated transition metals has enabled advanced processing and high minority carrier lifetimes in p-type mc-Si. This contribution extends that fundamental understanding to Fe contamination in n-type mc-Si, helping enable processing of this material into an economical and high-performance photovoltaic device. Finally, by directly correlating micro-photoluminescence-based minority carrier lifetime mapping and synchrotron-based micro-X-ray fluorescence mapping of Fe-rich precipitates, we develop a quantitative, physical understanding of the recombination activity of Fe-rich precipitates in n-type mc-Si.
36 MATERIALS SCIENCE↗
Utilization of Tabula Rasa to Stabilize Bulk Lifetimes in n-Cz Silicon for High-Performance Solar Cell Processing
We investigate a high temperature, high cooling-rate anneal Tabula Rasa (TR) and report its implications on n-type Czochralski-grown silicon (n-Cz Si) for photovoltaic fabrication. Tabula Rasa aims at dissolving and homogenizing oxygen precipitate nuclei that can grow during the cell process steps and degrade the cell performance due to their high internal gettering and recombination activity. The Tabula Rasa thermal treatment is performed in a clean tube furnace with cooling rates >100 degrees C/s. We characterize the bulk lifetime by Sinton lifetime and photoluminescence mapping just after Tabula Rasa, and after the subsequent cell processing. After TR, the bulk lifetime surprisingly degrades to <; 0.1ms, only to recover to values equal or higher than the initial non-treated wafer (several ms), after typical high temperature cell process steps. Those include boron diffusion and oxidation; phosphorus diffusion/oxidation; ambient annealing at 850 degrees C; and crystallization annealing of tunneling-passivating contacts (doped polycrystalline silicon on 1.5 nm thermal oxide). The drastic lifetime improvement during high temperature cell processing is attributed to improved external gettering of metal impurities and annealing of intrinsic point defects. Time and injection dependent lifetime spectroscopy further reveals the mechanisms of lifetime improvement after Tabula Rasa treatment. Additionally, we report the efficacy of Tabula Rasa on n-type Cz-Si wafers and its dependence on oxygen concentration, correlated to position within the ingot.
14 SOLAR ENERGY↗
Influence of oxygen vacancies on the domain wall stability in BiFeO 3
Oxygen vacancy is the most common type of point defects in functional oxides, and it is known to have profound influence on their properties. This is particularly true for ferroelectric oxides since their interaction with ferroelectric polarization often dictates the ferroelectric responses. Here, we study the influence of the concentration of oxygen vacancies on the stability of ferroelectric domain walls (DWs) in BiFeO 3 , a material with a relatively narrow bandgap among all perovskite oxides, which enables strong interactions among electronic charge carriers, oxygen vacancies, and ferroelectric domains. It is found that the electronic charge carriers in the absence of oxygen vacancies have essentially no influence on the spatial polarization distribution of the DWs due to their low concentrations. Upon increasing the concentration of oxygen vacancies, charge-neutral DWs with an originally symmetric polarization distribution symmetric around the center of the wall can develop a strong asymmetry of the polarization field, which is mediated by the electrostatic interaction between polarization and electrons from the ionization of oxygen vacancies. Strongly charged head-to-head DWs that are unstable without oxygen vacancies can be energetically stabilized in the off-stoichiometric BiFeO 3–δ with δ ~ 0.02 where ionization of oxygen vacancies provides sufficient free electrons to compensate the bound charge at the wall. Our results delineate the electrostatic coupling of the ionic defects and the associated free electronic charge carriers with the bound charge in the vicinity of neutral and charged DWs in perovskite ferroelectrics.
36 MATERIALS SCIENCE↗