Engineering topics

Graf, David

Publications and source records attributed to Graf, David.

At least 19 records

DOE OSTI2025

Enhancement of Superconductivity in WP via Oxide-Assisted Chemical Vapor Transport

Tungsten monophosphide (WP) has been reported to superconduct below 0.8 K, and theoretical work has predicted an unconventional Cooper pairing mechanism. Here we present data for WP single crystals grown by means of chemical vapor transport (CVT) of WO3, P, and I2. In comparison to synthesis using WP powder as a starting material, this technique results in samples with substantially decreased low-temperature scattering and favors a more three-dimensional morphology. We also find that the resistive superconducting transitions in these samples begin above 1 K. Variation in Tc is often found in strongly correlated superconductors, and its presence in WP could be the result of influence from a competing order and/or a non-s-wave gap.

Chemistry↗

DOE OSTI2024

Semi-Dirac Fermions in a Topological Metal

Topological semimetals with massless Dirac and Weyl fermions represent the forefront of quantum materials research. In two dimensions, a peculiar class of fermions that are massless in one direction and massive in the perpendicular direction was predicted 16 years ago. These highly exotic quasiparticles—the semi-Dirac fermions—ignited intense theoretical and experimental interest but remain undetected. Using magneto-optical spectroscopy, we demonstrate the defining feature of semi-Dirac fermions— B 2 / 3 scaling of Landau levels—in a prototypical nodal-line metal ZrSiS. In topological metals, including ZrSiS, nodal lines extend the band degeneracies from isolated points to lines, loops, or even chains in the momentum space. With calculations and theoretical modeling, we pinpoint the observed semi-Dirac spectrum to the crossing points of nodal lines in ZrSiS. Crossing nodal lines exhibit a continuum absorption spectrum but with singularities that scale as B 2 / 3 at the crossing. Our work sheds light on the hidden quasiparticles emerging from the intricate topology of crossing nodal lines and highlights the potential to explore quantum geometry with linear optical responses. Published by the American Physical Society 2024

Shao, Yinming (ORCID:0000000228910028)↗

DOE OSTI2024

Insulator‐to‐Metal Transition and Isotropic Gigantic Magnetoresistance in Layered Magnetic Semiconductors

Magnetotransport, the response of electrical conduction to external magnetic field, acts as an important tool to reveal fundamental concepts behind exotic phenomena and plays a key role in enabling spintronic applications. Magnetotransport is generally sensitive to magnetic field orientations. In contrast, efficient and isotropic modulation of electronic transport, which is useful in technology applications such as omnidirectional sensing, is rarely seen, especially for pristine crystals. Here a strategy is proposed to realize extremely strong modulation of electron conduction by magnetic field which is independent of field direction. GdPS, a layered antiferromagnetic semiconductor with resistivity anisotropies, supports a field-driven insulator-to-metal transition with a paradoxically isotropic gigantic negative magnetoresistance insensitive to magnetic field orientations. This isotropic magnetoresistance originates from the combined effects of a near-zero spin–orbit coupling of Gd 3+ -based half-filling ƒ-electron system and the strong on-site f – d exchange coupling in Gd atoms. These results not only provide a novel material system with extraordinary magnetotransport that offers a missing block for antiferromagnet-based ultrafast and efficient spintronic devices, but also demonstrate the key ingredients for designing magnetic materials with desired transport properties for advanced functionalities.

36 MATERIALS SCIENCE↗

DOE OSTI2024

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

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

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Absence of E 2 g Nematic Instability and Dominant A 1 g Response in the Kagome Metal CsV 3 Sb 5

Ever since the discovery of the charge density wave (CDW) transition in the kagome metal CsV 3 Sb 5 , the nature of its symmetry breaking has been under intense debate. While evidence suggests that the rotational symmetry is already broken at the CDW transition temperature ( T CDW ), an additional electronic nematic instability well below T CDW has been reported based on the diverging elastoresistivity coefficient in the anisotropic channel ( m E 2 g ). Verifying the existence of a nematic transition below T CDW is not only critical for establishing the correct description of the CDW order parameter, but also important for understanding low-temperature superconductivity. Here, we report elastoresistivity measurements of CsV 3 Sb 5 using three different techniques probing both isotropic and anisotropic symmetry channels. Contrary to previous reports, we find the anisotropic elastoresistivity coefficient m E 2 g is temperature independent, except for a step jump at T CDW . The absence of nematic fluctuations is further substantiated by measurements of the elastocaloric effect, which show no enhancement associated with nematic susceptibility. On the other hand, the symmetric elastoresistivity coefficient m A 1 g increases below T CDW , reaching a peak value of 90 at T * = 20 K . Our results strongly indicate that the phase transition at T * is not nematic in nature and the previously reported diverging elastoresistivity is due to the contamination from the A 1 g channel. Published by the American Physical Society 2024

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2024

Probing the van Hove singularity of the kagome metal YV 6 Sn 6 through quantum oscillations

Kagome metals with the Fermi energy tuned near the van Hove singularities (vHss) have shown to host exotic phases including unconventional superconductivity and a chiral flux phase arising from a charge density wave. However, most quantum oscillations studies of the electronic structure of kagome metals focus on compounds which electronically or magnetically order, obscuring the unperturbed vHs. Here we present quantum oscillation measurements of YV 6 ⁢Sn 6 which contains a pristine kagome lattice free from long-range order. We discovered quantum oscillations corresponding to a large orbit (≈70% of the Brillouin Zone area) with the heaviest mass ever observed in vanadium-based kagome metals (≈3.3⁢m e ), consistent with a Fermi pocket whose Fermi level is near the vHs. Comparing with first-principle calculations suggests that the effective mass of this pocket is highly sensitive to the position of Fermi level. Finally, our study establishes the enhanced density of states associated with a vHs in a kagome metal, allowing further insight into a potential driving mechanism for the unconventional electronic orderings in this class of materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

High-entropy engineering of the crystal and electronic structures in a Dirac material

Dirac and Weyl semimetals are a central topic of contemporary condensed matter physics, and the discovery of new compounds with Dirac/Weyl electronic states is crucial to the advancement of topological materials and quantum technologies. Here we show a widely applicable strategy that uses high configuration entropy to engineer relativistic electronic states. We take the A MnSb 2 ( A = Ba, Sr, Ca, Eu, and Yb) Dirac material family as an example and demonstrate that mixing of Ba, Sr, Ca, Eu and Yb at the A site generates the compound (Ba 0.38 Sr 0.14 Ca 0.16 Eu 0.16 Yb 0.16 )MnSb 2 (denoted as A 5 MnSb 2 ), giving access to a polar structure with a space group that is not present in any of the parent compounds. A 5 MnSb 2 is an entropy-stabilized phase that preserves its linear band dispersion despite considerable lattice disorder. Although both A 5 MnSb 2 and A MnSb 2 have quasi-two-dimensional crystal structures, the two-dimensional Dirac states in the pristine A MnSb 2 evolve into a highly anisotropic quasi-three-dimensional Dirac state triggered by local structure distortions in the high-entropy phase, which is revealed by Shubnikov–de Haas oscillations measurements.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Engineering Anomalously Large Electron Transport in Topological Semimetals

Abstract Anomalous transport of topological semimetals has generated significant interest for applications in optoelectronics, nanoscale devices, and interconnects. Understanding the origin of novel transport is crucial to engineering the desired material properties, yet their orders of magnitude higher transport than single‐particle mobilities remain unexplained. This work demonstrates the dramatic mobility enhancements result from phonons primarily returning momentum to electrons due to phonon‐electron dominating over phonon–phonon scattering. Proving this idea, proposed by Peierls in 1932, requires tuning electron and phonon dispersions without changing symmetry, topology, or disorder. This is achieved by combining de Haas ‐ van Alphen (dHvA), electron transport, Raman scattering, and first‐principles calculations in the topological semimetals MX 2 (M = Nb, Ta and X = Ge, Si). Replacing Ge with Si brings the transport mobilities from an order magnitude larger than single particle ones to nearly balanced. This occurs without changing the crystal structure or topology and with small differences in disorder or Fermi surface. Simultaneously, Raman scattering and first‐principles calculations establish phonon–electron dominated scattering only in the MGe 2 compounds. Thus, this study proves that phonon‐drag is crucial to the transport properties of topological semimetals and provides insight to engineer these materials further.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Two-dimensional heavy fermions in the van der Waals metal CeSiI

Heavy-fermion metals are prototype systems for observing emergent quantum phases driven by electronic interactions. A long-standing aspiration is the dimensional reduction of these materials to exert control over their quantum phases, which remains a significant challenge because traditional intermetallic heavy-fermion compounds have three-dimensional atomic and electronic structures. Here we report comprehensive thermodynamic and spectroscopic evidence of an antiferromagnetically ordered heavy-fermion ground state in CeSiI, an intermetallic comprising two-dimensional (2D) metallic sheets held together by weak interlayer van der Waals (vdW) interactions. Owing to its vdW nature, CeSiI has a quasi-2D electronic structure, and we can control its physical dimension through exfoliation. The emergence of coherent hybridization of f and conduction electrons at low temperature is supported by the temperature evolution of angle-resolved photoemission and scanning tunnelling spectra near the Fermi level and by heat capacity measurements. Electrical transport measurements on few-layer fakes reveal heavy-fermion behaviour and magnetic order down to the ultra-thin regime. Importantly, our work establishes CeSiI and related materials as a unique platform for studying dimensionally confined heavy fermions in bulk crystals and employing 2D device fabrication techniques and vdW heterostructures to manipulate the interplay between Kondo screening, magnetic order and proximity effects.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Coexistence of Dirac fermion and charge density wave in the square-net-based semimetal LaAuSb 2

Here, we report a comprehensive study of magnetotransport properties, angle-resolved photoemission spectroscopy (ARPES), and density functional theory (DFT) calculations on self-flux grown LaAuSb 2 single crystals. Resistivity and Hall measurements reveal a charge density wave (CDW) transition at 77 K. MR and de Haas-Van Alphen (dHvA) measurements indicate that the transport properties of LaAuSb 2 are dominated by Dirac fermions that arise from Sb square nets. ARPES measurements and DFT calculations reveal an electronic structure with a common feature of the square-net-based topological semimetals, which is in good agreement with the magnetotransport properties. Our results indicate the coexistence of CDW and Dirac fermion in LaAuSb 2 , both of which are linked to the bands arising from the Sb-square net, suggesting that the square net could serve as a structural motif to explore various electronic orders.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Large anomalous Hall effect and negative magnetoresistance in half-topological semimetals

Proposed mechanisms for large intrinsic anomalous Hall effect (AHE) in magnetic topological semimetals include diverging Berry curvatures of Weyl nodes, anticrossing nodal rings or points of non-trivial bands. Here we demonstrate that a half-topological semimetal (HTS) state near a topological critical point can provide an alternative mechanism for a large AHE via systematic studies on an antiferromagnetic (AFM) half-Heusler compound TbPdBi. We not only observe a large AHE with tanΘ H ≈ 2 in its field-driven ferromagnetic (FM) phase, but also find a distinct Hall resistivity peak in its canted AFM phase. Moreover, we observe a large negative magnetoresistance with a value of ~98%. Our in-depth theoretical modelling indicates that these exotic transport properties originate from the HTS state which exhibits Berry curvature cancellation between the trivial spin-up and nontrivial spin-down bands. Our study offers alternative strategies for improved materials design for spintronics and other applications.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Three-dimensional flat bands in pyrochlore metal CaNi 2

Electronic flat-band materials host quantum states characterized by a quenched kinetic energy. These flat bands are often conducive to enhanced electron correlation effects and emergent quantum phases of matter. Long studied in theoretical models, these systems have received renewed interest after their experimental realization in van der Waals heterostructures and quasi-two-dimensional (2D) crystalline materials. An outstanding experimental question is if such flat bands can be realized in three-dimensional (3D) networks, potentially enabling new materials platforms and phenomena. Here we investigate the C15 Laves phase metal CaNi 2 , which contains a nickel pyrochlore lattice predicted at a model network level to host a doubly-degenerate, topological flat band arising from 3D destructive interference of electronic hopping. Using angle-resolved photoemission spectroscopy, we observe a band with vanishing dispersion across the full 3D Brillouin zone that we identify with the pyrochlore flat band as well as two additional flat bands that we show arise from multi-orbital interference of Ni d -electrons. Furthermore, we demonstrate chemical tuning of the flat-band manifold to the Fermi level that coincides with enhanced electronic correlations and the appearance of superconductivity. Extending the notion of intrinsic band flatness from 2D to 3D, this provides a potential pathway to correlated behaviour predicted for higher-dimensional flat-band systems ranging from tunable topological to fractionalized phases.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Electronic transport and thermoelectricity in the selenospinel Cu 6—x Fe 4+x Sn 12 Se 32

Here, we report a study of selenospinel Cu 6—x Fe 4+x Sn 12 Se 32 (x = 0, 1, 2) single crystals, which crystallize in a cubic structure with the F$d$$\overline{3}$$m$ space group, and show typical semiconducting behavior. The large discrepancy between the activation energy for electrical conductivity E ρ (32.3–69.8 meV), and for thermopower E S (3.2–11.5 meV), indicates a polaronic transport mechanism between 350 and 50 K. With decreasing temperature, it evolves into variable-range hopping conduction. Furthermore, the heat capacity shows a hump around 25(5) K and diverges from the Debye T 3 law at low temperatures, indicating the observation of structural glassy features in these crystalline solids.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Revealing a 3D Fermi Surface Pocket and Electron-Hole Tunneling in UTe 2 with Quantum Oscillations

Spin triplet superconductor UTe 2 is widely believed to host a quasi-two-dimensional Fermi surface, revealed by first-principles calculations, photoemission and quantum oscillation measurements. An outstanding question still remains as to the existence of a three-dimensional Fermi surface pocket, which is crucial for our understanding of the exotic superconducting and topological properties of UTe 2 . This 3D Fermi surface pocket appears in various theoretical models with different physics origins, but has not been unambiguously detected in experiment. Here, in this study, for the first time we provide concrete evidence for a relatively isotropic, small Fermi surface pocket of UTe 2 via quantum oscillation measurements. In addition, we observed high frequency quantum oscillations corresponding to electron-hole tunneling between adjacent electron and hole pockets. The coexistence of 2D and 3D Fermi surface pockets, as well as the breakdown orbits, provides a test bed for theoretical models and aid the realization of a unified understanding of superconducting state of UTe 2 from the first-principles approach.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Robust three-dimensional type-II Dirac semimetal state in SrAgBi

Topological semimetals such as Dirac, Weyl or nodal line semimetals are widely studied for their peculiar properties including high Fermi velocities, small effective masses and high magnetoresistance. When the Dirac cone is tilted, exotic phenomena could emerge whereas materials hosting such states are promising for photonics and plasmonics applications. Here we present evidence that SrAgBi is a spin-orbit coupling-induced type-II three-dimensional Dirac semimetal featuring tilted Dirac cone at the Fermi energy. Near charge compensation and Fermi surface characteristics are not much perturbed by 7% of vacancy defects on the Ag atomic site, suggesting that SrAgBi could be a material of interest for observation of robust optical and spintronic topological quantum phenomena.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Beyond single tetrahedron physics of the breathing pyrochlore compound Ba 3 ⁢Yb 2 ⁢Zn 5 ⁢O 11

Recently, a new class of quantum magnets, the so-called breathing pyrochlore spin systems, have attracted much attention due to their potential to host exotic emergent phenomena. Here, we present magnetometry, heat capacity, thermal conductivity, muon-spin relaxation, and polarized inelastic neutron scattering measurements performed on high-quality single crystal samples of the breathing pyrochlore compound Ba 3 ⁢Yb 2 ⁢Zn 5 ⁢O 11 . We interpret these results using a simplified toy model and provide insight into the low-energy physics of this system beyond the single tetrahedron physics proposed previously.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Thermal transport properties of IrSbSe

Here we report a thermal transport study of IrSbSe, which crystallizes in a noncentrosymmetric cubic structure with the P2 1 3 space group and shows a narrow-gap semiconducting behavior. The large discrepancy between the activation energy for conductivity [E ρ = 128(2) meV] and for thermopower [E S = 17.7 (9) meV] from 200 to 300 K indicates a polaronic transport mechanism. The electrical resistivity varies as exp (T 0 /T) 1/4 and thermopower varies as T 1/2 at low temperatures, indicating that it evolves into Mott variable-range hopping dominant conduction with decreasing temperature. IrSbSe shows a relatively low value of thermal conductivity (~1.65 W/Km) and thermopower of about 0.24 mV/K around 100 K, yet poor electrical conductivity. On the other hand, a high vacancy defect concentration on both Ir and Sb atomic sites of up to 15% suggests a high defect tolerance and points to the possibility of a future improvement of carrier density by chemical substitution or defect optimization.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Quasi-two-dimensional Fermi surface of superconducting line-nodal metal CaSb 2

We report on the Fermi surfaces and superconducting parameters of CaSb 2 single crystals (superconducting below T c ~1.8K) grown by the self-flux method. The frequency of de Haas–van Alphen and Shubnikov–de Haas oscillations evidences a quasi-two-dimensional (quasi-2D) Fermi surface, consistent with one of the Fermi surfaces forming Dirac lines predicted by first-principles calculations. Measurements in the superconducting state reveal that CaSb 2 is close to a type-I superconductor with the Ginzburg-Landau parameter of around unity. The temperature dependence of the upper critical field H c2 is well described by a model considering two superconducting bands, and the enhancement of the effective mass estimated from H c2 (0K) is consistent with the quasi-2D band observed by the quantum oscillations. Our results indicate that a quasi-2D band forming Dirac lines contributes to the superconductivity in CaSb 2 .

36 MATERIALS SCIENCE↗