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At least 271 records · Page 15

Large non-saturating Nernst thermopower and magnetoresistance in compensated semimetal ScSb

Today, high-performance thermoelectric and thermomagnetic materials operating in the low-temperature regime, particularly below the boiling point of liquid nitrogen remain scarce. Most thermomagnetic materials reported to date exhibit a strong Nernst signal along specific crystallographic directions in their single-crystal form. However, their performance typically degrades significantly in the polycrystalline form. Here, we report an improved Nernst thermopower of ~ 128 μV/K at 30 K and 14 T in polycrystalline compensated semimetal ScSb, in comparison to that was observed in single crystal ScSb previously. The magnetic field dependence of Nernst thermopower shows a linear and non-saturating behavior up to 14 T. The maximum Nernst power factor reaches to ~ 240 x 10 -4 W m −1 K −2 and Nernst figure of merit reaches to ~ 11 x 10 -4 K −1 . Polycrystalline ScSb also shows a large non-saturating magnetoresistance of ~ 940% at 2 K and 14 T. These enhanced properties originate from better electron–hole compensation, as revealed by Hall resistivity measurements. In conclusion, the cubic symmetry and absence of anisotropy in ScSb allow its polycrystalline form to achieve similar enhanced thermomagnetic and electromagnetic performance comparable to that of the single crystal.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Lithium indium diselenide — An advanced material for neutron detection

Here, this paper describes the synthesis, crystal growth, detector fabrication, radiation hardening studies, MCNP modeling, and characterization of lithium indium diselenide or LiInSe 2 . This newly-developed room temperature thermal neutron detector has semiconducting and scintillating properties and it is suitable for neutron detection application. LiInSe 2 was synthesized starting from elemental Li, In, Se in two steps due to high reactivity of Li. A single crystal of LiInSe 2 was grown using the Vertical Bridgman method. The room temperature band gap was found to be 2.8 eV using optical absorption measurements. Bulk resistivity was measured at ∼5 × 10 11 Ωcm. Photoconductivity measurements of LiInSe 2 wafers identified a peak in the photocurrent around 445 nm. Nuclear radiation detectors were fabricated from single crystal wafer and the responses to alpha particles at various biases were measured. The mobility-lifetime product was estimated. Gamma irradiation studies were performed with calculated absorbed doses ranging from 0.2126 to 21,262 Gy. The characterization of the two wafers for their scintillator performance was conducted after each irradiation. The gamma irradiation produced a reduction of the light yield that translated to a lower channel number for the centroid of alpha detection spectra. It also showed a considerable reduction of the decay time after the first irradiation. These are the first studies on gamma radiation hardening with this material.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

A predictive analytical model of electrical transport in multi-principal-element alloys

A predictive analytical model is presented for the electrical conductivity of multi-principal-element alloys (MPEAs), including those containing aluminum, transition metals, and refractory metals. Given that the lattice parameter of the Wigner-Seitz cell of an MPEA is similarly variable to a bulk metallic glass, it is postulated that electron scattering can be approximated by a series of two-level systems. Here, the resulting reduced-order model enabled an accurate determination of electrical resistivity and electron thermal conductivity based on the scattering of electrons in a two-level system across a Bloch-potential-based virtual crystal approximation. Model results are compared to experimental four-point probe electrical resistivity measurements between 300 K and 700 K for Al 0.3 CoCrCuFeNi, CoCrFeMnNi, (CoCrFeMnNi) 0.98 W 0.02 , (CoCrFeMnNi) 0.95 W 0.05 , and Nb 4 Ta 4 V 3 Ti, for model validation.

Analytical model↗

Rapid characterization and failure analysis of 6276 rooftop-harvested photovoltaic connectors

Photovoltaic (PV) connectors, which link modules in series and connect PV strings in parallel, have increasingly been recognized as a primary contributor to PV system failures and a source of numerous fire incidents. However, publicly available data on the rates and types of connector failures are scarce, primarily due to the proprietary nature of the information and the need for comprehensive analysis. This study represents the first large-scale investigation of harvested PV connectors, drawing from a dataset of 6276 connectors from residential rooftop solar systems across the United States. The outcome of this work is twofold: 1) we have established a rapid characterization method for large populations of harvested connectors, incorporating visual inspection, resistance measurements, and X-ray imaging; and 2) the analysis made possible by our rapid-processing method has revealed, for a population of connector models provided by a single rooftop installer, failure statistics and insights for various connector makes and models, installation practices, operating currents, and internal component displacements. This research identifies common failure modes that could be considered in future connector designs standards, and operations and maintenance practices, to ultimately improve the reliability of this vital component of PV infrastructure.

MC4↗

Disorder driven variations in magnetoresistance and planar Hall effect in Bi 2 Te 3 thin films

The degenerately doped sesquichalcogenide Bi 2 Te 3 , a well-known thermoelectric material, has attracted much attention in recent years as a topological insulator in which conducting surface states lead to exotic electronic transport. Here, in this study, we report the observation of anisotropic magnetoresistance (AMR) and planar Hall effect (PHE) in polycrystalline thin films of Bi 2 Te 3 over a broad range of temperature and magnetic field strength. The values of AMR, PHE and the Hall mobility (μ H ) are compared with results of similar measurements on single crystals and epitaxial films of Bi 2 Te 3 , where these properties are understood in the framework of electronic transport in the topologically protected conducting surface states. Our textured polycrystalline films show a robust metallic character with a carrier density (n s ) and mobility μ H of 9×10 20 cm -3 and 16.7 cm 2 V -1 s -1 respectively. This carrier density is higher and the mobility lower by an order of magnitude compared to the reported values of n s and μ H in epitaxial films and single crystals. However, we see a comparable AMR and PHE in our films for which the concept of conducting surface states is ill-defined due to their polycrystallinity and disordered structure. We suggest that an anisotropic backscattering of charge carriers in the strongly spin – orbit coupled electronic states of this heavy-metal-based non-magnetic compound may lead to the measured resistivity anisotropy. The observation of AMR and PHE in polycrystalline films may be important for scalable production of Bi 2 Te 3 based AMR and PHE sensors of magnetic fields.

36 MATERIALS SCIENCE↗

Effect of substrate temperature on the growth of Nb 3 Sn film on Nb by multilayer sputtering

Here, we report on the fabrication of niobium tin (Nb 3 Sn) films by multilayer sequential sputtering on niobium at substrate temperatures ranging from room temperature to 250 °C. The multilayers were then annealed inside a separate vacuum furnace at 950 °C for 3 h. The material properties of the films were characterized by X-ray diffraction, scanning electron microscopy, energy-dispersive X-ray spectroscopy, atomic force microscopy, and transmission electron microscopy. The superconducting properties of the films were studied by four-point probe resistivity measurements from room temperature to below the superconducting critical temperature T c . The highest film T c was 17.76 K, obtained when the multilayers were deposited at room temperature. When the deposition temperature was raised to 250 °C, a significant reduction in voids was achieved while the film's T c was 17.58 K.

36 MATERIALS SCIENCE↗

Electrochemical-driven green recovery of lithium, graphite and cathode from lithium-ion batteries using water

The expected exponential increase in consumption of lithium-ion batteries (LIBs) would pose a unique challenge to the availability of near-critical resources like lithium and graphite in the upcoming decade. In this work, we present a lithium recovery process that utilizes a degradation mechanism, i.e., lithium plating, as a tool to concentrate metallic lithium at the anode/separator interface for convenient extraction at room temperature – using only water. Electrochemical characterization of fast charged (1–6 C) LIBs yielded a maximum capacity fade of 50% over ten cycles. The lithium plating was confirmed via voltage plateau analysis, coulombic efficiency, and DC resistance measurements. A maximum lithium plating condition was observed to exist between 4C and 5C, thereby limiting the energy consumption in the extraction process. Post-mortem film thickness measurement showed an incrementing film deposition with a maximum of 35 µm thickness. SEM and XPS analysis confirmed increasing concentration of a dense dendritic metallic lithium deposition on the anode/separator interface with C-rate. A green recovery process was adopted to extract the concentrated metallic lithium using distilled water. The lithium from the plated film, solid/electrolyte interface (SEI), electrolyte, anode, and cathode, was extracted as salts. A 37% improvement in lithium recoverability was achieved with fast charging under ambient conditions. XPS analysis showed ~92% of lithium yield with no residual lithium in the graphite. In addition, the battery-grade graphite was recovered with 97% purity after heat treatment of the washed anode film, and concentrated transition metals oxides in the cathode to 93% purity for convenient extraction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Structure, Magnetism, and First-Principles Modeling of the Na 0.5 La 0.5 RuO 3 Perovskite

High-purity polycrystalline Na 0.5 La 0.5 RuO 3 was synthesized by a solid-state method, and its properties were studied by magnetic susceptibility, heat capacity, and resistivity measurements. In this study, we find it to be an orthorhombic perovskite, in contrast to an earlier report, with random La/Na mixing. With a Curie–Weiss temperature of –231 K and an effective moment of 2.74 μB/mol Ru, there is no magnetic ordering down to 1.8 K. A broad hump at 1.4 K in the heat capacity, however, indicates the presence of a glassy magnetic transition, which we attribute to the influence of the random distribution of Na and La on the perovskite A-sites. Comparison to CaRuO 3 , a structurally ordered ruthenate perovskite with a similar A-site ionic radius and magnetic properties, is presented. First-principles calculations indicate that the Na–La distribution determines the local magnetic exchange interactions between Ru ions, favoring either antiferromagnetic or ferromagnetic coupling when the local environment is Na- or La-rich. Thus, our data and analysis suggest that mixing cations with different charges and sizes on the A-site in this perovskite results in magnetic frustration through a balance of local magnetic exchange interactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Local Distortions and Metal–Semiconductor–Metal Transition in Quasi-One-Dimensional Nanowire Compounds AV 3 Q 3 O δ (A = K, Rb, Cs and Q = Se, Te)

Metal cluster compounds have garnered renewed interest in the search for novel superconductors and topological semimetals owing to structural instabilities of metal-cluster geometries and broken symmetries. Here we synthesized needle-like crystals of the V-cluster-based quasi-one-dimensional (Q1D) materials AV 3 Q 3 O δ (A = K, Rb, Cs, Q= Se, Te) which can also be viewed as being composed of parallel nanowires. We examine how changes in their average and local structure control their electronic properties. All compounds crystallize in the TIFe 3 Te 3 -type structure (P6 3 /m space group) with infinite (V 3 )Q 3 ) - double-walled columnar chains separated by A + cations. Our single-crystal and synchrotron powder diffraction studies indicate oxygen atoms partially occupy the center site of the V 6 octahedral metal cluster cages in KV 3 Te 3 O 0.33 , RbV 3 Te 3 O 0.32 , and CsV 3 Te 3 O 0.35 , whereas KV 3 Se 3 is structurally oxygen-free. Our synchrotron X-ray pair distribution function (PDF) analyses indicate that the oxygen-free V 6 cluster octahedra in KV 3 Se 3 are highly distorted perpendicular to the chain direction even at room temperature, reducing the symmetry of the average structure from hexagonal P6 3 /m to monoclinic P2 1 /m. Our theoretical calculation supports this P2 1 /m distortion and suggests the structure further distorts to P2 1 or P2 1 /c at lower temperatures. In contrast, the oxygen-centered V-cluster in KV 3 Te 3 O 0.33 exhibits a V-3-triangle-trimerization along the chain direction. This feature is discernible from the local PDF and is consistent with lattice dynamical calculations based on density functional theory. Resistivity measurements indicate that KV 3 Se 3 exhibits metallic behavior, whereas a dramatic metal-semiconductor-metal transition emerges in KV 3 Te 3 O 6.33 , RbV 3 Te 3 O 0.32 , and CsV 3 Te 3 O 0.35 because of oxygen disorder and changes in local structure captured from our electronic structure analyses of the Fermi surface. Our investigation of the AV 3 Q 3 O 6 family demonstrates the importance of understanding local changes in structure driven by electronic instabilities, which can guide the search for new quantum materials in other low-dimensional cluster-compound materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Flux Growth of Cerium Nickel Gallides Studied by In Situ Neutron Diffraction

In this work, reactions of cerium and nickel in excess molten gallium were monitored by neutron diffraction during heating and cooling. The formation of binary intermediates CeGa 2 and Ni 2 Ga 3 was observed during heating. During cooling of the molten mixture from 900 °C, precipitation of BaAl 4 -type CeNi 0.74 Ga 3.26 occurred at 850 °C. Upon cooling to 650 °C, this compound reacted in the flux to form Ce 2 NiGa 10 and then Ce 2 NiGa 12 , the latter of which persisted to room temperature. Making use of this information, subsequent reactions were quenched at 750 °C to isolate crystals of CeNi 0.74 Ga 3.26 for further study. Similar reactions replacing Ce with La and quenching above 750 °C yielded LaNi 0.35 Ga 3.65 crystals. Magnetic susceptibility studies on CeNi 0.74 Ga 3.26 indicate that the cerium is trivalent; the Ce 3+ moments undergo a strongly anisotropic ferromagnetic ordering with moment perpendicular to the c axis below 7 K. Heat capacity data show little evidence of heavy fermion behavior. Resistivity measurements show that both LaNi0.35Ga3.65 and CeNi 0.74 Ga 3.26 exhibit metallic behavior. Density of states calculations support this and indicate that Ni/Ga mixing in the compound stabilizes the structure.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Non-Centrosymmetric Sr 2 IrO 4 Obtained Under High Pressure

Sr 2 IrO 4 with strong spin-orbit coupling (SOC) and Hubbard repulsion (U) hosts Mott insulating states. The similar crystal structure, magnetic and electronic properties, particularly the d-wave gap observed in Sr 2 IrO 4 enhanced the analogies to cuprate high-$T_c$ superconductor, La 2 CuO 4 . The incomplete analogy was due to the lack of broken inversion symmetry phases observed in Sr 2 IrO 4 . Here, under high pressure and high temperature conditions, we report a non-centrosymmetric Sr 2 IrO 4 . The crystal structure and its noncentrosymmetric character were determined by single crystal X-ray diffraction and high-resolution scanning transmission electron microscopy (HR-STEM). The magnetic characterization confirms the Ir 4+ with $\textit{S}$ = 1/2 at low temperature in Sr 2 IrO 4 with magnetic ordering occurred at around 86 K, where a larger moment is observed than the ambient pressure Sr 2 IrO 4 . Moreover, the resistivity measurement shows three-dimensional Mott variable-range hopping existed in the system. Further, this non-centrosymmetric Sr 2 IrO 4 phase appears to be a unique material to offer further understanding of high-$T_c$ superconductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Synthesis of Layered Gold Tellurides AuSbTe and Au 2 Te 3 and Their Semiconducting and Metallic Behavior

Previous studies on natural samples of pampaloite (AuSbTe) revealed the crystal structure of a potentially cleavable and/or exfoliable material, while studies on natural and synthetic montbrayite (Sb-containing Au 2 Te 3 ) claimed various chemical compositions for this low-symmetry compound. Few investigations of synthetic samples have been reported for both materials, leaving much of their chemical, thermal, and electronic characteristics unknown. Here, in this study, we investigate the stability, electronic properties, and synthesis of the gold antimony tellurides AuSbTe and Au 1.9 Sb 0.46 Te 2.64 (montbrayite). Differential thermal analysis and in situ powder X-ray diffraction revealed that AuSbTe is incongruently melting, while Au 1.9 Sb 0.46 Te 2.64 is congruently melting. Calculations of the band structures and four-point resistivity measurements showed that AuSbTe is a semiconductor and Au 1.9 Sb 0.46 Te 2.64 a metal. Various synthesis attempts confirmed the limited stable chemical composition of Au 1.9 Sb 0.46 Te 2.64 , identified successful methods to synthesize both compounds, and highlighted the challenges associated with single-crystal synthesis of AuSbTe.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Charge Carrier Transport in Iron Pyrite Thin Films: Disorder-Induced Variable-Range Hopping

Here, the origin of p-type conductivity and the mechanism responsible for low carrier mobility were investigated in pyrite (FeS 2 ) thin films. Temperature-dependent resistivity measurements (10-400 K) were performed on polycrystalline and nanostructured thin films prepared by three different methods: (1) spray pyrolysis, (2) hot-injection synthesized and spin-coated nanocubes, and (3) pulsed laser deposition. The films have a high hole density (10 18 -10 19 ) cm -3 and low mobility (0.1-4 cm 2 V -1 s -1 ) regardless of the method used for their preparation. The charge transport mechanism is determined to be thermally activated conduction (TAC) at near room temperature, with Mott-type variable-range hopping (VRH) of holes via localized states occurring at lower temperatures. The density functional theory (DFT) predicts that sulfur vacancy induces localized defect states within the band gap and the charge remains localized around the defect. The data indicates that the electronic properties including hopping transport in pyrite thin films can be correlated to sulfur vacancy-related defects. The results provide insights into the electronic properties of pyrite thin films and their implications for charge transport.

36 MATERIALS SCIENCE↗

Evidence of a coupled electron-phonon liquid in NbGe 2

Whereas electron-phonon scattering relaxes the electron’s momentum in metals, a perpetual exchange of momentum between phonons and electrons may conserve total momentum and lead to a coupled electron-phonon liquid. Such a phase of matter could be a platform for observing electron hydrodynamics. Here we present evidence of an electron-phonon liquid in the transition metal ditetrelide, NbGe 2 , from three different experiments. First, quantum oscillations reveal an enhanced quasiparticle mass, which is unexpected in NbGe 2 with weak electron-electron correlations, hence pointing at electron-phonon interactions. Second, resistivity measurements exhibit a discrepancy between the experimental data and standard Fermi liquid calculations. Third, Raman scattering shows anomalous temperature dependences of the phonon linewidths that fit an empirical model based on phonon-electron coupling. We discuss structural factors, such as chiral symmetry, short metallic bonds, and a low-symmetry coordination environment as potential design principles for materials with coupled electron-phonon liquid.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Creating superconductivity in WB 2 through pressure-induced metastable planar defects

High-pressure electrical resistivity measurements reveal that the mechanical deformation of ultra-hard WB 2 during compression induces superconductivity above 50 GPa with a maximum superconducting critical temperature, T c of 17 K at 91 GPa. Upon further compression up to 187 GPa, the T c gradually decreases. Theoretical calculations show that electron-phonon mediated superconductivity originates from the formation of metastable stacking faults and twin boundaries that exhibit a local structure resembling MgB 2 (hP3, space group 191, prototype AlB 2 ). Synchrotron x-ray diffraction measurements up to 145 GPa show that the ambient pressure hP12 structure (space group 194, prototype WB 2 ) continues to persist to this pressure, consistent with the formation of the planar defects above 50 GPa. The abrupt appearance of superconductivity under pressure does not coincide with a structural transition but instead with the formation and percolation of mechanically-induced stacking faults and twin boundaries. The results identify an alternate route for designing superconducting materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Electronic properties of the bulk and surface states of Fe 1+y Te 1-x Se x

The idea of employing non-Abelian statistics for error-free quantum computing ignited interest in reports of topological surface superconductivity and Majorana zero modes (MZMs) in FeTe 0.55 Se 0.45 . However, the topological features and superconducting properties are not observed uniformly across the sample surface. The understanding and practical control of these electronic inhomogeneities present a prominent challenge for potential applications. Here, we combine neutron scattering, scanning angle-resolved photoemission spectroscopy, and microprobe composition and resistivity measurements to characterize the electronic state of Fe 1+y Te 1-x Se x . Furthermore, we establish a phase diagram in which the superconductivity is observed only at sufficiently low Fe concentration, in association with distinct antiferromagnetic correlations, whereas the coexisting topological surface state occurs only at sufficiently high Te concentration. We find that FeTe 0.55 Se 0.45 is located very close to both phase boundaries, which explains the inhomogeneity of superconducting and topological states. Our results demonstrate the compositional control required for use of topological MZMs in practical applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Unconventional unidirectional magnetoresistance in heterostructures of a topological semimetal and a ferromagnet

Unidirectional magnetoresistance (UMR) in a bilayer heterostructure, consisting of a spin-source material and a magnetic layer, refers to a change in the longitudinal resistance on the reversal of magnetization and originates from the interaction of non-equilibrium spin accumulation and magnetization at the interface. Since the spin polarization of an electric-field-induced non-equilibrium spin accumulation in conventional spin-source materials is restricted to be in the film plane, the ensuing UMR can only respond to the in-plane component of magnetization. However, magnets with perpendicular magnetic anisotropy are highly desired for magnetic memory and spin-logic devices, whereas the electrical read-out of perpendicular magnetic anisotropy magnets through UMR is critically missing. Here, in this study, we report the discovery of an unconventional UMR in the heterostructures of a topological semimetal (WTe 2 ) and a perpendicular magnetic anisotropy ferromagnetic insulator (Cr 2 Ge 2 Te 6 ), which allows to electrically read the up and down magnetic states of the Cr 2 Ge 2 Te 6 layer through longitudinal resistance measurements.

Kao, I-Hsuan [Carnegie Mellon Univ., Pittsburgh, P↗

Pressure-tuned plethora of ferroelectric phases in CuInP 2 S 6

Layered chalcogenides like CuInP 2 S 6 are room temperature ferroelectrics. Modest compression even increases the electric polarization, raising questions about the origin of this unusual trend and other properties under pressure. In this work, we combine synchrotron-based infrared and Raman scattering spectroscopies, x-ray diffraction, and resistivity measurements with first-principles calculations of the lattice dynamics and energy landscape to unravel the influence of pressure on symmetry, polarization, and metallicity. We uncover a remarkable series of phase transitions across a series of polar space groups: monoclinic Cc → trigonal P31c (prismatic sulfur) → P31c (octahedral sulfur). True metallicity develops above 63 GPa, significantly higher than in related MPS 3 materials (M = Mn, Co, Fe, Ni), offering a picture of competing states of matter that is different than previously supposed. Detailed examination of pressure trends within the Cc phase also reveals phonon lifetime changes and streaking of satellite x-ray peaks that correlate with the maximum polarization. We discuss these tendencies in terms of Cu + ion migration, phase formation, and the overall energy landscape. Our findings place the high pressure behavior of CuInP 2 S 6 on a firm foundation and pave the way for the development of structure-property relations in this family of complex chalcogenides.

ferroelectric phases↗