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At least 541 records · Page 30
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

To grind or not to grind? The influence of mechanical and thermal treatments on the $\mathrm{Cu/Zn}$ disorder in $\mathrm{Cu}$ 2 $\mathrm{ZnSn}$($\mathrm{S}$ x $\mathrm{Se}$ 1-x ) 4 monograins

We report that Kesterite-type based thin film solar cell technologies are mainly based on polycrystalline absorber layers. A promising low cost alternative technology uses Cu 2 ZnSn(S x Se 1-x ) 4 (CZTSSe) monograins (single crystals of 20–100 μm size) which are fixed in a polymer matrix to form a flexible solar cell. The Cu/Zn disorder is discussed as a possible reason for band tailing causing voltage losses limiting the efficiency of CZTSSe-based devices. The experimental determination of the order parameter Q which is a quantitative measure of Cu/Zn disorder, requires a differentiation between the isoelectronic cations Cu + and Zn 2+ . An in-depth analysis of neutron diffraction data allows the determination of type and concentration of intrinsic point defects including a distinction between Cu and Zn. Neutron diffraction requires large sample volumes, thus monograins offer the unique possibility to correlate structural disorder in CZTSSe with device performance parameters. In this study we tackle the influence of grinding the monograins on stoichiometry deviations, the Cu/Zn disorder as well as intrinsic point defects and optoelectronic properties of CZTSSe monograins. Moreover, an easy methodology based on Raman scattering spectroscopy is proposed for the assessment of Cu/Zn disorder in the CZTSSe compounds.

14 SOLAR ENERGY↗
DOE OSTI2022

Unusual electronic transport in (1 - x )Cu 2 Se-( x )CuInSe 2 hierarchical composites

The ability to control the relative density of electronic point defects as well as their energy distribution in semiconductors could afford a systematic modulation of their electronic, optical, and optoelectronic properties. Using a model binary hybrid system Cu 2 Se–CuInSe 2 , we have investigated the correlation between phase composition, microstructure, and electronic transport behavior in the synthesized composites. We found that both Cu 2 Se and CuInSe 2 phases coexist at multiple length scales, ranging from sub-ten nanometer to several micrometers, leading to the formation of a hybrid hierarchical microstructure. Astonishingly, the electronic phase diagram of the (1 - x)Cu 2 Se–(x)CuInSe 2 (15% ≤ x ≤ 100%) hierarchical composites remarkably deviates from the trend normally expected for composites between a heavily doped semiconductor (Cu 2 Se) and a poorly conducting phase (CuInSe 2 ). A sudden 3-fold increase in the electrical conductivity and carrier concentration along with a marginal increase in the carrier mobility is observed for composites at the vicinity of equimolar composition (48% ≤ x ≤ 52%). The carrier concentration increases from ~1.5 × 10 20 cm -3 for the composites with x ≤ 45% to 5.0 × 10 20 cm -3 for x = 50%, and remains constant at 4.5 × 10 20 cm -3 with x value in the range of 52% < x ≤ 90%, then quickly drops to 8 × 10 18 cm -3 for pristine CuInSe 2 phase (x = 100%). The atypical electronic behavior was rationalized in the light of the formation of an inter-band (IB) within the band gap, which arises from the hybridization of native electronic point defects from both Cu 2 Se and CuInSe 2 phases in the resulting hierarchical composites. The result points to a new strategy to modulate the electronic structure of semiconductor composites to maximize interaction and coupling between two fundamentally contrasting properties enabling access to electronic hybrid systems with potential applications as interactive and stimuli-responsive multifunctional materials.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Analysis of differential scanning calorimetry data for aged plutonium

Differential scanning calorimetry data for samples of a 52 year old plutonium alloy with 3.3 at. % Ga that were heated beyond the melting point is analyzed using transition state theory to find activation energies for the δ to ε and ε to liquid phase transitions. A Bayesian statistical method involving a Gaussian process model is used to find mean values and confidence intervals for the activation energies. The activation energy for the δ to ε phase transition increases by 3.3 ± 3.8% per decade, relative to the case when all age related plutonium lattice point defects have been removed through annealing. The corresponding increase in activation energy for the ε to liquid transition is shown to be 7.1 ± 1.8% per decade. It is postulated that the change in activation energy with age for both phase transitions is caused, in part, by the accumulation of the same type of lattice point defects associated with the observed increase in elastic bulk modulus over time.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Imaging atomic-scale effects of high-energy ion irradiation on superconductivity and vortex pinning in Fe(Se,Te)

Maximizing the sustainable supercurrent density, J C , is crucial to high-current applications of superconductivity, and to achieve this, preventing dissipative motion of quantized vortices is key. Irradiation of superconductors with highenergy heavy ions can be used to create nanoscale defects that act as deep pinning potentials for vortices. This approach holds unique promise for high-current applications of iron-based superconductors because JC amplification persists to much higher radiation doses than in cuprate superconductors without significantly altering the superconducting critical temperature. However, for these compounds, virtually nothing is known about the atomic-scale interplay of the crystal damage from the high-energy ions, the superconducting order parameter, and the vortex pinning processes. We visualize the atomic-scale effects of irradiating FeSe x Te 1$-$x with 249-MeV Au ions and find two distinct effects: compact nanometer-sized regions of crystal disruption or “columnar defects,” plus a higher density of single atomic site “point” defects probably from secondary scattering. We directly show that the superconducting order is virtually annihilated within the former but suppressed by the latter. Simultaneous atomically resolved images of the columnar crystal defects, the superconductivity, and the vortex configurations then reveal how amixed pinning landscape is created, with the strongest pinning occurring at metallic core columnar defects and secondary pinning at clusters of point-like defects, followed by collective pinning at higher fields.

Critical Current by Design↗
DOE OSTI2012

Low energy electron beam induced vacancy activation in GaN

Experimental evidence on low energy electron beam induced point defect activation in GaN grown by metal-organic vapor phase epitaxy (MOVPE) is presented. The GaN samples are irradiated with a 5-20 keV electron beam of a scanning electron microscope and investigated by photoluminescence and positron annihilation spectroscopy measurements. The degradation of the band-to-band luminescence of the irradiated GaN films is associated with the activation of point defects. The activated defects were identified as in-grown Ga-vacancies. We propose that MOVPE-GaN contains a significant concentration of passive V{sub Ga}-H{sub n} complexes that can be activated by H removal during low energy electron irradiation.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Solubility and Diffusivity: Important Metrics in the Search for the Root Cause of Light- and Elevated Temperature-Induced Degradation

Light- and elevated temperature-induced degradation (LeTID) is a detrimental effect observed under operating conditions in p-type multicrystalline silicon (mc-Si) solar cells. In this paper, we employ synchrotron-based techniques to study the dissolution of precipitates due to different firing processes at grain boundaries in LeTID-affected mc-Si. The synchrotron measurements show clear dissolution of collocated metal precipitates during firing. We compare our observations with degradation behavior in the same wafers. The experimental results are complemented with process simulations to provide insight into the change in bulk point defect concentration due to firing. Several studies have proposed that LeTID is caused by metal-rich precipitate dissolution during contact firing, and we find that the solubility and diffusivity are promising screening metrics to identify metals that are compatible with this hypothesis. While slower and less soluble elements (e.g., Fe and Cr) are not compatible according to our simulations, the point defect concentrations of faster and more soluble elements (e.g., Cu and Ni) increase after a high-temperature firing process, primarily due to emitter segregation rather than precipitate dissolution. Finally, these results are a useful complement to lifetime spectroscopy techniques, and can be used to evaluate additional candidates in the search for the root cause of LeTID.

14 SOLAR ENERGY↗
DOE OSTI2019

Impact of irradiation induced dislocation loops on thermal conductivity in ceramics

Experimental work aimed at understanding the role of dislocation loops in limiting phonon mediated thermal transport in ceramics is presented. Faulted dislocation loops, having diameters of a few nanometers, were introduced by irradiating a polycrystalline cerium dioxide sample with 1.6 MeV protons at 700°C. XRD analysis indicated that irradiated samples retained their crystalline structure and exhibit very little lattice expansion suggesting a low concentration of point defects. Additionally, further microstructure characterization using transmission electron microscopy revealed that interstitial type faulted dislocation loops were primarily created as expected for these irradiation conditions. Thermal conductivity of the damaged layer was measured using a modulated thermoreflectance approach. Analysis of the experimental data using the classical Klemens-Callaway approach reveals that the conductivity reduction is primarily due to dislocation loops, while point defects and voids play only a minor role. These results provide experimental confirmation that faulted loops offer a unique arrangement for displaced atoms that leads to an unusually large reduction of thermal conductivity.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Total dose effect of Al 2 O 3 -based metal–oxide–semiconductor structures and its mechanism under gamma-ray irradiation

In our work, insights into the total dose response and native point defect behavior in the Al2O3 gate dielectric during irradiation were gained by gamma-ray irradiation experiments and first-principles calculations. It is found that the O vacancy (VO) can act as a hole trap in the Al2O3 gate dielectric during irradiation, leading to the negative shift of the capacitance–voltage (C–V) curves of the Al2O3-based metal–oxide–semiconductor (MOS) structure. Our calculations show that the neutral defect VO becomes a +2 charged center after irradiation, and the positively charged VO is a kind of conductive path for electrons, which contributes to an increase of the leakage current in the irradiated MOS capacitors. Additionally, the trapped holes are accumulated with irradiation doses, which can lower the barrier height of the Al2O3 gate oxide and further cause the increase of the leakage current. The other native point defects in the Al2O3 layer, such as aluminum vacancy (VAl), aluminum interstitial (Ali) and oxygen interstitial (Oi), only act as fixed charge centers during irradiation. Net negative charges existing in the Al2O3 layers before irradiation are mainly induced by the negatively charged defects of VAl and Oi.

Engineering↗
DOE OSTI2018

Role of Sink Density in Nonequilibrium Chemical Redistribution in Alloys

Nonequilibrium chemical redistribution in open systems submitted to external forces, such as particle irradiation, leads to changes in the structural properties of the material, potentially driving the system to failure. Such redistribution is controlled by the complex interplay between the production of point defects, atomic transport rates, and the sink character of the microstructure. In this work, we analyze this interplay by means of a kinetic Monte Carlo (KMC) framework with an underlying atomistic model for the Fe-Cr model alloy to study the effect of ideal defect sinks on Cr concentration profiles, with a particular focus on the role of interface density. We observe that the amount of segregation decreases linearly with decreasing interface spacing. Within the framework of the thermodynamics of irreversible processes, a general analytical model is derived and assessed against the KMC simulations to elucidate the structure-property relationship of this system. Interestingly, in the kinetic regime where elimination of point defects at sinks is dominant over bulk recombination, the solute segregation does not directly depend on the dose rate but only on the density of sinks. Furthermore, this model provides new insight into the design of microstructures that mitigate chemical redistribution and improve radiation tolerance.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Thermodynamically Driven Formation of Intercalated Cu Carpets from Supported Cu Pyramids on MoS 2

Thermodynamic and kinetic analyses based on our first-principles density functional theory calculations are used to interpret the experimentally observed formation of Cu carpets intercalated under the top layer of a 2H-MoS 2 substrate. Spontaneous Cu transport from Cu pyramids on top of the MoS 2 substrate through surface point defects to the growing Cu carpet is shown to be driven by a slightly lower chemical potential for the Cu carpet. We demonstrate that the competition between a preference for a thicker Cu carpet and the cost of elastic stretching of the top MoS 2 layer results in a selected Cu carpet thickness. Furthermore, we also propose that Cu transport occurs primarily via vacancy-mediated diffusion through constricting point defect portals.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Screening mechanisms at polar oxide heterointerfaces

The interfaces of polar oxide heterostructures can display electronic properties unique from the oxides they border, as they require screening from either internal or external sources of charge. The screening mechanism depends on a variety of factors, including the band structure at the interface, the presence of point defects or adsorbates, whether or not the oxide is ferroelectric, and whether or not an external field is applied. In this review, we discuss both theoretical and experimental aspects of different screening mechanisms, giving special emphasis to ways in which the mechanism can be altered to provide novel or tunable functionalities. We begin with a theoretical introduction to the problem and highlight recent progress in understanding the impact of point defects on polar interfaces. Different case studies are then discussed, for both the high thickness regime, where interfaces must be screened and each interface can be considered separately, and the low thickness regime, where the degree and nature of screening can be manipulated and the interfaces are close enough to interact. As a result, we end with a brief outlook toward new developments in this rapidly progressing field.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Transition metal impurities in silicon: computational search for a semiconductor qubit

Abstract Semiconductors offer a promising platform for physical implementation of qubits, but their broad adoption is presently hindered by limited scalability and/or very low operating temperatures. Learning from the nitrogen-vacancy centers in diamond, our goal is to find equivalent optically active point defect centers in crystalline silicon, which could be advantageous for their scalability and integration with classical devices. Transition metal (TM) impurities in silicon are common paramagnetic deep defects, but a comprehensive theoretical study of the whole 3 d series that considers generalized Koopmans’ condition is missing. We apply the HSE06(+U) method to examine their potential as optically active spin qubits and identify seven TM impurities that have optically allowed triplet–triplet transitions within the silicon band gap. These results provide the first step toward silicon-based qubits with higher operating temperatures for quantum sensing. Additionally, these point defects could lead to spin-photon interfaces in silicon-based qubits and devices for mid-infrared free-space communications.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Phase-field modeling of radiation-induced composition redistribution: An application to additively manufactured austenitic Fe–Cr–Ni

Multicomponent alloys undergoing irradiation damage develop radiation-induced composition redistribution at point defect sinks such as grain boundaries (GBs) and dislocations. Such redistribution results in undesired changes to their mechanical behavior and corrosion resistance. Additively manufactured alloys proposed for future nuclear applications are expected to demonstrate a distinct response to irradiation owing to their unique microstructure with as-solidified dislocation density and chemical microsegregation. To capture the composition redistribution in such systems, we develop a mesoscale model with coupled evolution of atomic and point defect components in the presence of dislocation density, dislocation heterogeneity, and thermodynamic interactions at the GB. The model is parameterized for an FCC Fe–Cr–Ni alloy as a representative system for austenitic stainless steels, and simulations are performed in 1D and 2D as a function of irradiation temperature, dose, dislocation density, and grain size. Radiation-induced segregation (RIS) characterized by Cr depletion and Ni enrichment is predicted at both the GB and the dislocation cell wall, with RIS being lower in magnitude but wider at the cell wall. Strongly biased absorption of self-interstitials by dislocations is found to suppress Ni enrichment but slightly enhance Cr depletion under certain conditions. Thermodynamic segregation at the GB is predicted to be narrower and opposite in sign to RIS for both Cr and Ni. Importantly, non-monotonic segregation is found to occur when both thermodynamic and RIS mechanisms are considered, providing a novel physical interpretation of experimental observations. The model is expected to serve as a key tool in accelerated qualification of irradiated materials.

additively manufactured microstructure↗
DOE OSTI2016

SU-F-T-166: On the Nature of the Background Visible Light Observed in Fiber Optic Dosimetry of Proton Beams

Purpose: The nature of the background visible light observed during fiber optic dosimetry of proton beams, whether it is due to Cherenkov radiation or not, has been debated in the literature recently. In this work, experimentally and by means of Monte Carlo simulations, we shed light on this problem and investigated the nature of the background visible light observed in fiber optics irradiated with proton beams. Methods: A bare silica fiber optics was embedded in tissue-mimicking phantoms and irradiated with clinical proton beams with energies of 100–225 MeV at Roberts Proton Therapy Center. Luminescence spectroscopy was performed by a CCD-coupled spectrograph to analyze in detail the emission spectrum of the fiber tip across the visible range of 400–700 nm. Monte Carlo simulation was performed by using FLUKA Monte Carlo code to simulate Cherenkov light and ionizing radiation dose deposition in the fiber. Results: The experimental spectra of the irradiated silica fiber shows two distinct peaks at 450 and 650 nm, whose spectral shape is different from that of Cherenkov radiation. We believe that the nature of these peaks are connected to the point defects of silica including oxygen-deficiency center (ODC) and non-bridging oxygen hole center (NBOHC). Monte Carlo simulations confirmed the experimental observations that Cherenkov radiation cannot be solely responsible for such a signal. Conclusion: We showed that Cherenkov radiation is not the dominant visible signal observed in bare fiber optics irradiated with proton beams. We observed two distinct peaks at 450 and 650 nm whose nature is connected with the point defects of silica fiber including oxygen-deficiency center and non-bridging oxygen hole center.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2017

Lattice Dislocations Enhancing Thermoelectric PbTe in Addition to Band Convergence

Phonon scattering by nanostructures and point defects has become the primary strategy for minimizing the lattice thermal conductivity (κ L ) in thermoelectric materials. However, these scatterers are only effective at the extremes of the phonon spectrum. Recently, it has been demonstrated that dislocations are effective at scattering the remaining mid-frequency phonons as well. In this work, by varying the concentration of Na in Pb 0.97 Eu 0.03 Te, it has been determined that the dominant microstructural features are point defects, lattice dislocations, and nanostructure interfaces. This study reveals that dense lattice dislocations (≈4 × 10 12 cm -2 ) are particularly effective at reducing κ L . When the dislocation concentration is maximized, one of the lowest κ L values reported for PbTe is achieved. Furthermore, due to the band convergence of the alloyed 3% mol. EuTe the electronic performance is enhanced, and a high thermoelectric figure of merit, zT, of ≈2.2 is achieved. This work not only demonstrates the effectiveness of dense lattice dislocations as a means of lowering κL, but also the importance of engineering both thermal and electronic transport simultaneously when designing high-performance thermoelectrics.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Overcoming the doping limit in GaAs by ion implantation and pulsed laser melting

Most semiconductors exhibit a saturation of free carriers when heavily doped with extrinsic dopants. This carrier saturation or “doping limit” is known to be related to the formation of native compensating defects, which, in turn, depends on the energy positions of their conduction band minimum and valence band maximum. Here, we carried out a systematic study on the n-type doping limit of GaAs via ion implantation and showed that this doping limitation can be alleviated by the transient process of pulsed laser melting (PLM). For n-type doping, both group VI (S) and amphoteric group IV (Si and Ge) dopants were implanted in GaAs. For comparison, p-type doping was also studied using Zn as the acceptor. Implanted dopants were activated by the PLM method, and the results are compared to rapid thermal annealing (RTA). Our results reveal that for all n-type dopants, while implantation followed by the RTA results in a similar saturation electron concentration of 2–3 × 10 18 cm –3 , the transient PLM process is capable of trapping high concentration of dopants in the substitutional site, giving rise to a carrier concentration of >10 19 cm –3 , exceeding the doping limit of GaAs. However, due to scatterings from point defects generated during PLM, the mobility of n-type GaAs after PLM is low (~80–260 cm 2 /V s). Subsequent RTA after PLM (PLM + RTA) is able to remove these point defects and recover the mobility to ~1000–2000 cm2/V s. The carrier concentrations of these PLM + RTA samples are reduced but are still a factor of 3 higher than RTA only GaAs. This can be understood as the dopants are already incorporated in the substitutional site after PLM; they are less likely to be “deactivated” by subsequent RTA. This work is significant to the understanding of doping mechanisms in semiconductors and provides a means for device applications, which require materials with ultra-high doping.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Real-space representation of the quasiparticle self-consistent GW self-energy and its application to defect calculations

The quasiparticle self-consistent (QS) GW (G for Green's function, W for screened Coulomb interaction) approach incorporates the corrections of the quasiparticle energies from their Kohn-Sham density functional theory (DFT) eigenvalues by means of an energy-independent and Hermitian self-energy matrix usually given in the basis set of the DFT eigenstates. By expanding these into an atom-centered basis set (specifically here the linearized muffin-tin orbitals) a real space representation of the self-energy corrections becomes possible. In this work, We show that this representation is relatively short-ranged. This offers opportunities to construct the self-energy of a complex system from parts of the system by a cut-and-paste method. Specifically for a point defect, represented in a large supercell, the self-energy can be constructed from those of the host and a smaller defect-containing cell. The self-energy of the periodic host can be constructed simply from a GW calculation for the primitive cell. We show for the case of the As Ga in GaAs that the defect part can already be well represented by a minimal eight-atom cell and allows us to construct the self-energy for a 64-atom cell in good agreement with direct QSGW calculations for the large cell. Using this approach to an even larger 216-atom cell shows the defect band approaches an isolated defect level. The calculations also allow us to identify a second defect band which appears as a resonance near the conduction band minimum. The results on the extracted defect levels agree well with Green's function calculations for an isolated defect and with experimental data.

36 MATERIALS SCIENCE↗
DOE OSTI2013

The effect of structural vacancies on the thermoelectric properties of (Cu₂Te){sub 1–x}(Ga₂Te₃) x

We have studied the effects of structural vacancies on the thermoelectric properties of the ternary compounds (Cu₂Te) 1–x (Ga₂Te₃) x (x=0.5, 0.55, 0.571, 0.6, 0.625, 0.667 and 0.75), which are solid solutions found in the pseudo-binary phase diagram for Cu₂Te and Ga₂Te₃, and possesses tunable structural vacancy concentrations. This materials system is not suitable due to the cost and scarcity of the constituent elements, but the vacancy behavior is well understood and will provide a valuable test case for other systems more suitable from the standpoint of cost and abundance of raw materials, which also possesses these vacancy features, but whose structural characterization is lacking at this stage. We find that the nominally defect free phase CuGaTe₂ possess the highest ZT (ZT=S²T/ρκ, where S is the Seebeck coefficient and ρ is the electrical resistivity κ is the thermal conductivity and T is the absolute temperature) which approaches 1 at 840 K and seems to continuously increase above this temperature. This result is due to the unexpectedly low thermal conductivity found for this material at high temperature. The low thermal conductivity was caused by strong Umklapp (thermally resistive scattering processes involving three phonons) phonon scattering. We find that due to the coincidentally strong scattering of carriers by the structural defects that higher concentrations of these features lead to poor electrical transport properties and decreased ZT. - Graphical abstract: Thermal conductivity and zT as a function of temperature for a series of compounds of the type (Cu₂Te) 1–x (Ga₂Te₃)x (x=0.5, 0.55, 0.571, 0.6, 0.625, 0.667 and 0.75). Highlights: • All the samples show p-type semiconducting behavior in the temperature dependence of the Seebeck and Hall coefficients. • The increased carrier concentration and the introduction of vacancies diminish the carrier mobility and power factor. • The low temperature k decreases significantly as the Ga₂Te₃ content increases due to increasing point defects. • The highest ZT ~ 1.0 at 840 K among the samples in this study was found in CuGaTe₂, which contains no vacancies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗