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At least 91 records · Page 5

Effect of realistic out-of-plane dopant potentials on the superfluid density of overdoped cuprates

Recent experimental papers on hole-doped overdoped cuprates have argued that a series of observations showing unexpected behavior in the superconducting state imply the breakdown of the quasiparticle-based Landau–BCS paradigm in that doping range. In contrast, some of the present authors have argued that a phenomenological “dirty d-wave” theoretical analysis explains essentially all aspects of thermodynamic and transport properties in the superconducting state, provided the unusual effects of weak, out-of-plane dopant impurities are properly accounted for. Here we attempt to place this theory on a more quantitative basis by performing ab initio calculations of dopant impurity potentials for LSCO and Tl-2201. These potentials are more complex than the pointlike impurity models considered previously, and require calculation of forward scattering corrections to transport properties. Including realistic, ARPES-derived band structures, Fermi liquid renormalizations, and vertex corrections, we show that the theory can explain semiquantitatively the unusual superfluid density measurements of the two most studied overdoped materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Carbon-related donor–acceptor pair transition in the infrared in h-BN

Experimental studies of intentionally doped impurities for the understanding of conductivity control in hexagonal boron nitride (h-BN) ultrawide bandgap (UWBG) semiconductor are limited but are highly desired for emerging applications of h-BN. We report synthesis by hydride vapor phase epitaxy and comparison photoluminescence (PL) emission spectroscopy studies of intentionally carbon (C)-doped and undoped h-BN semi-bulk crystals. In addition to the well-known C-related emission lines observed previously, a C-impurity-related transition near 1.31 eV consisting of multiple phonon replicas has been observed in C-doped h-BN at room temperature. Phonon replicas involved in the 1.31 eV emission have been identified using polarization resolve PL spectroscopy as the transverse acoustic (TA)/longitudinal acoustic (LA) and out-of-plane optical phonon (ZO) modes at the middle point, T, between the Γ- and K-points in the first Brillouin zone. Based on the agreement between the spectral peak position of the observed dominant emission line at 1.31 eV and the calculated energy-level separation between CB donor (carbon replacing boron) and Ci acceptor (carbon interstitial), the observed IR emission line can be decisively assigned to the donor–acceptor pair (DAP) transition involving the CB donor and Ci acceptor assisted by the intervalley (Κ → Μ) scattering processes. The results reinforce the perception that C impurities form deep-level centers and provided an improved understanding of C impurities in h-BN.

Physics↗

Application of the portable diagnostic package to the Wisconsin high-temperature-superconducting axisymmetric mirror (WHAM)

We present an application of the Portable Diagnostic Package (PDP) on the Wisconsin High-temperature-superconducting Axisymmetric Mirror (WHAM), which integrates an optical emission spectroscopy (OES) system and an active Thomson scattering (TS) system. The OES system facilitates a comprehensive impurity line survey and enables flow measurements through the Doppler effect observed on impurity lines. Plasma rotation profiles were successfully derived from doubly charged carbon lines. The TS system enabled the first measurements of the electron temperature in commissioning plasmas on WHAM. Notably, the PDP was installed, commissioned, and used to obtain OES and TS data within ∼6 months from project start, enabled by its designed portability and standardized interfaces. These results demonstrate the PDP’s potential to accelerate diagnostic readiness and advance experimental plasma studies.

Doppler effect↗

Magnetic and transport properties of Fe-doped Weyl semimetal Co 3 Sn 2 S 2

Ferromagnetic Weyl semimetal Co 3 Sn 2 S 2 has recently attracted a lot of interest on account of its large non-saturating magnetoresistance and the high carrier mobility common to topological semimetals. Moreover, the material also provides a platform for studying the interplay between the intrinsic magnetism and topological band structures, which generates a significant anomalous Hall effect. Chemical doping is the usual approach to adjust materials’ properties, and it can lead to fascinating results. Here, we present the influence of Fe-doping on the magnetic and transport properties of polycrystalline Co 3 Sn 2 S 2 . The Fe-doping suppresses the sample’s magnetic order, increases the electrical resistivity, results in a skew-scattering contribution to the anomalous Hall effect and Fe impurities cause the Kondo effect. In addition, we report on the impact of Fe-doping on the magnetoresistance of Co 3 Sn 2 S 2 , where Fe-doping leads to a dramatic decline in magnetoresistance. Furthermore, the hysteresis behavior in the low magnetic field region, detected previously in nanoflake samples only, is observed in both pure and Fe-doped Co 3 Sn 2 S 2 bulk samples. Finally, our findings serve as a reference and source of inspiration for future chemical doping research on topological semimetals.

36 MATERIALS SCIENCE↗

Optimal carrier concentration for FeSb 2 colossal thermopower

Crystals of FeSb 2 correlated narrow-gap semiconductor host colossal thermopower values. By tuning the impurity level here, we demonstrate that electron-phonon scattering that transfers phonon momentum to electrons is efficient only for certain optimal carrier concentration in the low-mobility band. Phonon drag acting on such states in crystals with high phonon mean free path enhances thermopower to colossal values, whereas for different carrier concentration, dominant thermal transport mechanism is electronic diffusion. This highlights the dual nature of correlated in-gap states that take part in the phonon drag but also reduce phonon mean free path.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Electronic Band Structure of a Superconducting Nickelate Probed by the Seebeck Coefficient in the Disordered Limit

Superconducting nickelates are a new family of strongly correlated electron materials with a phase diagram closely resembling that of superconducting cuprates. While analogy with the cuprates is natural, very little is known about the metallic state of the nickelates, making these comparisons difficult. We probe the electronic dispersion of thin-film superconducting five-layer ( n = 5 ) and metallic three-layer ( n = 3 ) nickelates by measuring the Seebeck coefficient S . We find a temperature-independent and negative S / T for both n = 5 and n = 3 nickelates. These results are in stark contrast to the strongly temperature-dependent S / T measured at similar electron filling in the cuprate La 1.36 Nd 0.4 Sr 0.24 CuO 4 . The electronic structure calculated from density-functional theory can reproduce the temperature dependence, sign, and amplitude of S / T in the nickelates using Boltzmann transport theory. This demonstrates that the electronic structure obtained from first-principles calculations provides a reliable description of the fermiology of superconducting nickelates and suggests that, despite indications of strong electronic correlations, there are well-defined quasiparticles in the metallic state. Finally, we explain the differences in the Seebeck coefficient between nickelates and cuprates as originating in strong dissimilarities in impurity concentrations. Our study demonstrates that the high elastic scattering limit of the Seebeck coefficient reflects only the underlying band structure of a metal, analogous to the high magnetic field limit of the Hall coefficient. This opens a new avenue for Seebeck measurements to probe the electronic band structures of relatively disordered quantum materials. Published by the American Physical Society 2024

Grissonnanche, G. (ORCID:0000000251153125)↗

Suppression of thermal conductivity and electronic correlations in Fe 1– x Ru x Sb 2 (0 ≤ x ≤ 0.6)

We present simultaneous suppression of FeSb 2 thermal conductivity and electronic correlations in Fe 1– x Ru x Sb 2 (0 ≤ x ≤ 0.6) single crystal alloys. Small energy gap Δ 1 in Kondo-insulator-like semiconductor FeSb 2 associated with impurity in-gap state increases whereas the intrinsic bandgap Δ 2 decreases upon Ru substitution on Fe atomic site. Thermopower is suppressed along with the intrinsic bandgap and with the thermal conductivity. The more delocalized 4 d character of atomic orbital of Ru brings suppression of electronic correlations, but also an increase in impurity density which reduces phonon mean free path and surface scattering length. Our results indicate a range of Ru doping x where nanostructuring could be used to suppress thermal conductivity further, potentially toward the amorphous limit.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Enhanced hydrodynamic transport in near magic angle twisted bilayer graphene

Using the semiclassical quantum Boltzmann theory and employing the Dirac model with twist angle-dependent Fermi velocity, we obtain results for the electrical resistivity, the electronic thermal resistivity, the Seebeck coefficient, and the Wiedemann-Franz ratio in near magic angle twisted bilayer graphene, as functions of doping density (around the charge-neutrality point) and modified Fermi velocity $\tilde{v}$. The $\tilde{v}$ dependence of the relevant scattering mechanisms, i.e., electron-hole Coulomb, long-range impurities, and acoustic gauge phonons, is considered in detail. We find a range of twist angles and temperatures, where the combined effect of momentum-nonconserving collisions (long-range impurities and phonons) is minimal, opening a window for the observation of strong hydrodynamic transport. In this work, several experimental signatures are identified, such as a sharp dependence of the electric resistivity on doping density and a large enhancement of the Wiedemann-Franz ratio and the Seebeck coefficient.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Portable diagnostic package for Thomson scattering and optical emission spectroscopy on Princeton field-reversed configuration 2 (PFRC 2)

An Advanced Research Projects Agency-Energy funded diagnostic system has been deployed to the Princeton field-reversed configuration 2 (PFRC-2) device, located at Princeton Plasma Physics Laboratory. The Portable Diagnostic Package (PDP), designed at Oak Ridge National Laboratory, allows for the measurement of Thomson Scattering (TS) for electron density and temperature and Optical Emission Spectroscopy (OES) for ion temperature, impurity density, and ion velocity. A tunable spectrometer on the PDP with three gratings provides the flexibility to measure low (1 eV) and high (1000 eV) electron temperature ranges from TS. Additionally, using a second spectrometer, the OES diagnostic can survey light emission from various ion excitation levels for wide wavelength ranges. The electron density (<2 × 10 19 m –3 ) of plasmas generated in PFRC-2 has been below the PDP TS discrimination threshold, which has made TS signal detection challenging against a high-background of laser stray light. The laser stray light was iteratively reduced by making modifications to the entrance and exit geometry on PFRC-2. Rayleigh scattering experiments on PFRC have yielded the TS discrimination sensitivity to be >1 × 10 20 m –3 for the PDP. A recently implemented narrow-band notch spectral filter that masks the second harmonic 532 nm Nd:YAG laser wavelength has increased the system’s TS light discrimination sensitivity 65 times compared to the instance when the notch filter was not implemented. The hardware implementation including design changes to the flight tubes and Brewster windows will be discussed, along with results from Rayleigh and rotational Raman scattering sensitivity analyses, which were used to establish a quantitative figure of merit on the system performance. Further, the Raman scattering calibration with the notch filter has improved the PDP electron density threshold to 1 ± 0.5 × 10 18 m –3 .

47 OTHER INSTRUMENTATION↗

Understanding how minority relativistic electron populations may dominate charge state balance and radiative cooling of a post-thermal quench tokamak plasma

Minority relativistic electron populations can occur in a range of complex plasmas. Of specific interest is when runaway electrons form among the presence of high-atomic-number ion species in a tokamak plasma discharge. It has been recently demonstrated that ion charge state distributions and radiation losses at low bulk electron temperatures can be dominated by relativistic electrons, even though their density is orders of magnitude lower. Furthermore, this was attributed to the relativistic enhancement of electron impact inelastic cross sections. In this work, we provide a closer inspection of the atomic physics underpinning this effect. We also demonstrate the consequences of runaway enhanced scattering on post-disruption tokamak fusion discharges with neon and argon impurities present. Effects on charge state distributions, radiation and spectral characteristics, and reduced-order modeling considerations are discussed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Errors introduced in fission neutron spectrum measurements using a single reference

Measurements of physical quantities are often made relative to a reference quantity, simplifying the interpretation of the measurement and its uncertainties. However, if applied without careful considerations, this technique can carry with it a significant and complex systematic error that is usually ignored. For example, measurements of continuous neutron spectra relative to a reference spectrum yield a result that does not properly include the important effects of neutron scattering in the experimental environment. These effects act to distort the measured spectrum shape and create notable errors in spectrum-integrated quantities. While this effect is one of a series of known potential sources of systematic error including, but not limited to target impurities, angular distributions, incident beam flux, and others, the error introduced from differences in environmental scattering effects between the reference and desired spectra are frequently overlooked. In this work, we demonstrate the origin of this error using simulated data corresponding to measurements of the neutron-induced prompt fission neutron spectra of 233 U, 235 U, 238 U, and 239 Pu as well as the spontaneous fission neutron spectrum of 252 Cf. Errors in the spectrum shape can be as high as 10%–15% depending on the combination of incident and outgoing neutron energy. The spectrum integral and average spectrum energy also contain errors that change with incident neutron energy and can be as high as ~2%. Although this study is based on simulated data, we also show a method for proving that this error exists in an experimental data set and we show a correction that can be applied to results of this type to obtain a more accurate result, thereby largely removing systematic errors from environmental scattering effects. The potential for these kinds of errors should be considered in measurements producing continuous neutron spectra.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

From weak antilocalization to Kondo scattering in a magnetic complex oxide interface

Quantum corrections to electrical resistance can serve as sensitive probes of the magnetic landscape of a material. For example, interference between time-reversed electron paths gives rise to weak localization effects, which can provide information about the coupling between spins and orbital motion, while the Kondo effect is sensitive to the presence of spin impurities. In this work, we use low-temperature magnetotransport measurements to reveal a gradual transition from weak antilocalization (WAL) to Kondo scattering in the quasi-two-dimensional electron gas formed at the interface between SrTiO 3 and the Mott insulator NdTiO 3 . This transition occurs as the thickness of the NdTiO 3 layer is increased. Analysis of the Kondo scattering and WAL points to the presence of atomic-scale magnetic impurities coexisting with nanoscale magnetic regions that affect transport via a strong magnetic exchange interaction. This leads to distinct magnetoresistance behaviors that can serve as a sensitive probe of magnetic properties in two dimensions.

36 MATERIALS SCIENCE↗

Enhanced Electron-Phonon Coupling for Charge-Density-Wave Formation in La 1.8-$x$ Eu 0.2 Sr $x$ CuO 4+$δ$

Charge density wave (CDW) correlations are prevalent in all copper-oxide superconductors. While CDWs in conventional metals are driven by coupling between lattice vibrations and electrons, the role of the electron-phonon coupling (EPC) in cuprate CDWs is strongly debated. Using Cu L 3 edge resonant inelastic x-ray scattering, we study the CDW and Cu-O bond-stretching phonons in the stripe-ordered cuprate La 1.8-x Eu 0.2 Sr x CuO 4+δ . In this work, we investigate the interplay between charge order and EPC as a function of doping and temperature and find that the EPC is enhanced in a narrow momentum region around the CDW ordering vector. By detuning the incident photon energy from the absorption resonance, we extract an EPC matrix element at the CDW ordering vector of M ≃ 0.36 eV , which decreases to M ≃ 0.30 eV at high temperature in the absence of the CDW. Our results suggest a feedback mechanism in which the CDW enhances the EPC which, in turn, further stabilizes the CDW.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Grain boundary widening controls siderite (FeCO3) replacement of limestone (CaCO3)

Abstract The microstructure of minerals and rocks can significantly alter reaction rates. This study focuses on identifying transport paths in low porosity rocks based on the hypothesis that grain boundary widening accelerates reactions in which one mineral is replaced by another (replacement reaction). We conducted a time series of replacement experiments of three limestones (CaCO 3 ) of different microstructures and solid impurity contents using FeCl 2 . Reacted solids were analyzed using chemical imaging, small angle X-ray and neutron scattering and Raman spectroscopy. In high porosity limestones replacement is reaction controlled and complete replacement was observed within 2 days. In low porosity limestones that contain 1–2% dolomite impurities and are dominated by grain boundaries, a reaction rim was observed whose width did not change with reaction time. Siderite (FeCO 3 ) nucleation was observed in all parts of the rock cores indicating the percolation of the solution throughout the complete core. Dolomite impurities were identified to act as nucleation sites leading to growth of crystals that exert force on the CaCO 3 grains. Widening of grain boundaries beyond what is expected based on dissolution and thermal grain expansion was observed in the low porosity marble containing dolomite impurities. This leads to a self-perpetuating cycle of grain boundary widening and reaction acceleration instead of reaction front propagation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Fundamental chemical physics revealed by scattering reactive open-shell atoms from surfaces

The dynamics of reactive atoms at surfaces are centrally important to areas such as heterogeneous catalysis, corrosion, materials degradation in extreme environments, and plasma etching. Remarkably detailed understanding of dynamical processes at surfaces has been extracted from scattering molecules and inert atoms under well-defined conditions. However, traditional techniques for generating beams of reactive atoms often result in impure mixtures, broad energy distributions, and poorly defined contributions of metastable electronically excited atoms. In this perspective article, we review the state-of-the-art in reactive atom surface scattering with a focus on experiments performed under controlled conditions on well-defined surfaces. We highlight a new technique for controlled state-to-state scattering of polyelectronic atoms from surfaces, based on vacuum ultraviolet photolysis and state-selective ion imaging. The new capabilities provide an avenue for research into the underexplored area of excited state and spin selective chemical dynamics at surfaces.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Effect of Impurities on the Redox Properties of Goethite

Iron oxide minerals regulate the flux of electrons in the environment and are important hosts for trace and minor, yet critical, elements. Here, we present the first evidence of a direct link between the local coordination environments of Ni and Zn and the redox properties of their host phase goethite (α-FeOOH), the most abundant Fe(III) (oxyhydr)oxide at Earth’s surface. Here, we used aqueous redox measurements to show that the redox potential E H 0 , and hence the mineral’s stability, follows the order: pure goethite ≥ Zn-goethite > Ni-goethite. Parallel X-ray absorption and scattering measurements demonstrate, using quantum-informed analysis, that the local coordination environment of the smaller impurity, Ni, causes more bulk strain energy than Zn, which nearly accounts for the difference in E H 0 between Ni- and Zn-goethite. Our theory-informed, experimental study reveals how two common impurities affect the stability of goethite with implications for the biogeochemical reactivity of Fe(III) (oxyhydr)oxide in mediating elemental and electron fluxes in the environment.

42 ENGINEERING↗

Single crystal growth of iridates without platinum impurities

Iridates have attracted much interest in the last decade for their novel magnetism emerging in the limit of strong spin-orbit coupling and possible unconventional superconductivity. A standard for growing iridate single crystals has been the flux method using platinum crucibles. Here, in this work, we show that this widely used method compromises the sample quality by inclusion of platinum impurities. We find that Sr 2 ⁢IrO 4 single crystals grown in iridium crucibles show remarkable differences from those grown in platinum crucibles in their sample characterizations using Raman spectroscopy, resistivity, magnetization, optical third harmonic generation, resonant x-ray diffraction, and resonant inelastic x-ray scattering measurements. In particular, we show that several peaks of sizable intensities disappear in the Raman spectra of samples free of platinum impurities, and a significantly larger activation energy is extracted from the resistivity data compared to previously reported values. Furthermore, we find no evidence of the previously reported glide-symmetry-breaking structural distortions and confirm the I⁢ 4 1 / acd space group of the lattice symmetry. Although the platinum impurities are not apparent in the magnetic properties and thus went unnoticed in the stoichiometric insulating phase for a long time, their effects can be much more detrimental to transport properties in chemically doped compounds. Therefore, our result suggests using growth methods that avoid platinum impurities for an investigation of the intrinsic physical properties of iridates, and possible superconducting phases.

36 MATERIALS SCIENCE↗