arXiv subjects

Tyrel M. McQueen

Publications and source records attributed to Tyrel M. McQueen.

At least 37 records · Page 2Linked to original sources

arXiv2024

Unmasking charge transfer in the Misfits: ARPES and ab initio prediction of electronic structure in layered incommensurate systems without artificial strain

Common belief is that the large band shifts observed in incommensurate misfit compounds, e.g. (LaSe)1.14(NbSe2)2, are due to interlayer charge transfer. In contrast, our analysis, based on both ARPES measurements and a specialized ab initio framework employing only quantities well defined in incommensurate materials, demonstrates that the large band shifts instead reflect changes in valence band hybridization and interlayer bonding. The strong alignment of our ab initio predictions and ARPES measurements confirms our understanding of the incommensurate electronic structure and charge transfer.

cond-mat.mtrl-sci↗

arXiv2024

Quasi-one-dimensional exchange interactions and short-range magnetic correlations in CuTeO4

CuTeO4 has been proposed as a crystallographically distinct, yet electronic structure analog, of the superconducting cuprates. Here, we present detailed characterization of the of the physical properties of CuTeO4 to address this proposal. Fitting of magnetic susceptibility data indicates unexpected quasi-one-dimensional, antiferromagnetic correlations at high temperature, with a nearest neighbour Heisenberg exchange of J1=165(4) K. Low temperature heat capacity measurements reveal a sizable T-linear contribution of $γ= 9.58(8) mJ mol^{-1} K^{-2}$, qualitatively consistent with expectations for a S=1/2, uniform, Heisenberg spin chain. Below T ~ 40 K, the susceptibility shows an upturn inconsistent with quasi-one-dimensional behaviour. While heat capacity measurements show no signs of magnetic order down to low temperature, the upturn in the magnetic susceptibility coincides with the emergence of a diffuse peak (centered at |Q| ~ 0.7 Angstrom) in the neutron diffraction data, indicative of persistent, short-range, antiferromagnetic order with a correlation length of $ξ$ = 10.1(9) Angstrom at T = 10 K. The onset of nonlinearity and hysteresis in the isothermal magnetization curves suggest the presence of a small ferromagnetic component. This persistent, short-range order is understood in the context of structural modeling of the x-ray and neutron diffraction data that show the presence of a significant density of stacking faults. No evidence for substantive dopability is observed and CuTeO4 appears qualitatively, to have a larger band gap than predicted by density functional theory. We ascribe this finding to the inductive withdrawal effect from high-valence Te and suggest that superconductivity in the copper tellurates is more likely to be found in compounds with a decreased reductive withdrawal effect from Te.

cond-mat.str-el↗

arXiv2024

Rashba spin splitting-induced topological Hall effect in a Dirac semimetal-ferromagnetic semiconductor heterostructure

We use a concerted theory-experiment effort to investigate the formation of chiral real space spin texture when the archetypal Dirac semimetal Cd$_3$As$_2$ is interfaced with In$_{1-x}$Mn$_x$As, a ferromagnetic semiconductor with perpendicular magnetic anisotropy. Our calculations reveal a nonzero off-diagonal spin susceptibility in the Cd$_3$As$_2$ layer due to the Rashba spin-orbit coupling from broken inversion symmetry. This implies the presence of a Dzyaloshinskii-Moriya interaction between local moments in the In$_{1-x}$Mn$_x$As layer, mediated by Dirac electrons in the vicinal Cd$_3$As$_2$ layer, potentially creating the conditions for a real space chiral spin texture. Using electrical magnetoresistance measurements at low temperature, we observe an emergent excess contribution to the transverse magneto-resistance whose behavior is consistent with a topological Hall effect arising from the formation of an interfacial chiral spin texture. This excess Hall voltage varies with gate voltage, indicating a promising electrostatically-tunable platform for understanding the interplay between the helical momentum space states of a Dirac semimetal and chiral real space spin textures in a ferromagnet.

cond-mat.mes-hall↗

arXiv2024

Hydroflux-Controlled Growth of Magnetic K-Cu-Te-O(H) Phases

Innovative synthetic approaches can yield new phases containing novel structural and magnetic motifs. In this work, we show the synthesis and magnetic characterization of three new and one previously reported layered phase in the K-Cu-Te-O(H) phase space using a tunable hydroflux technique. The hydroflux, with a roughly equal molar ratio of water and alkali hydroxide, is a highly oxidizing, low melting solvent which can be used to isolate metastable phases unattainable through traditional solid state or flux techniques. The newly synthesized phases, K$_{2}$Cu$_{2}$TeO$_{6}$, K$_{2}$Cu$_{2}$TeO$_{6}$ $\cdot$ H$_{2}$O, and K$_{6}$Cu$_{9}$Te$_{4}$O$_{24}$ $\cdot$ 2 H$_{2}$O, contain Cu$^{2+}$ within CuO$_{4}$ square planar plaquettes and TeO$_{6}$ octahedra ordering to form structural honeycomb layers isolated by interlayer K$^{+}$ ions and H$_{2}$O molecules. We find the synthesized structures display varying tilt sequences of the CuO$_{4}$ plaquettes, leading to distinct Cu$^{2+}$ magnetic motifs on the structural honeycomb lattice and a range of effective magnetic dimensionalities. We find that K$_{2}$Cu$_{2}$TeO$_{6}$ $\cdot$ H$_{2}$O does not order and displays alternating chain Heisenberg antiferromagnetic (AFM) behavior, while K$_{2}$Cu$_{2}$TeO$_{6}$ and K$_{6}$Cu$_{9}$Te$_{4}$O$_{24}$ $\cdot$ 2 H$_{2}$O order antiferromagnetically (T$_{N}$ = 100 K and T$_{N}$ = 6.5 K respectively). The previously known phase, K$_{2}$CuTeO$_{4}$(OH)$_{2}$ $\cdot$ H$_{2}$O, we find contains structurally and magnetically one-dimensional CuO$_{4}$ plaquettes leading to uniform chain Heisenberg AFM behavior and shows no magnetic order down to T = 0.4 K. We discuss and highlight the usefulness of the hydroflux technique in novel syntheses and the interesting magnetic motifs that arise in these particular phases.

cond-mat.str-el↗

arXiv2024

Quantum Fluctuations Suppress the Critical Fields in BaCo$_2$(AsO$_4$)$_2$

Early efforts to realize exotic quantum ground states in frustrated magnets focused on frustration arising from the lattice geometry alone. Attention has shifted to bond-dependent anisotropic interactions, as well as further-neighbor interactions, on non-geometrically-frustrated lattices due to their greater versatility. The honeycomb magnet BaCo$_2$(AsO$_4$)$_2$ recently emerged as a candidate host for both bond-dependent (e.g. Kitaev) and third-neighbor ($J_3$) interactions, and has become a model experimental system due to its relatively low levels of disorder. Understanding the relative importance of different exchange interactions holds the key to achieving novel ground states, such as quantum spin liquids. Here, we use the magnetotropic susceptibility to map out the intermediate and high-field phase diagram of BaCo$_2$(AsO$_4$)$_2$ as a function of the out-of-plane magnetic field direction at $T = 1.6$ K. We show that the experimental data are qualitatively consistent with classical Monte Carlo results of the XXZ-$J_1$-$J_3$ model with small Kitaev and off-diagonal exchange couplings included. However, the calculated critical fields are systematically larger than the experimental values. Infinite-DMRG computations on the quantum model reveal that quantum corrections from a nearby ferromagnetic state are likely responsible for the suppressed critical fields. Together, our experiment and theory analyses demonstrate that, while quantum fluctuations play an important role in determining the phase diagram, most of the physics of BaCo$_2$(AsO$_4$)$_2$ can be understood in terms of the classical dynamics of long-range ordered states, leaving little room for the possibility of a quantum spin liquid.

cond-mat.str-el↗

arXiv2023

Non-collinear 2k antiferromagnetism in the Zintl semiconductor Eu$_5$In$_2$Sb$_6$

Eu$_5$In$_2$Sb$_6$ is an orthorhombic non-symmorphic small band gap semiconductor with three distinct Eu$^{2+}$ sites and two low-temperature magnetic phase transitions. The material displays one of the greatest (negative) magnetoresistances of known stoichiometric antiferromagnets and belongs to a family of Zintl materials that may host an axion insulator. Using single crystal neutron diffraction, we show that the $T_{\mathrm{N1}}=14\mathrm{~K}$ second-order phase transition is associated with long-range antiferromagnetic order within the chemical unit cell $\left( k_1 = (000) \right)$. Upon cooling below $T_{\mathrm{N1}}$, the relative sublattice magnetizations of this structure vary until a second-order phase transition at $T_{\mathrm{N2}}=7\mathrm{~K}$ that doubles the unit cell along the $\hat{c}$ axis $\left( k_2 = \left(00\frac{1}{2}\right) \right)$. We show the anisotropic susceptibility and our magnetic neutron diffraction data are consistent with magnetic structures described by the $Γ_3$ irreducible representation with the staggered magnetization of the $k_1$ and $k_2$ components polarized along the $\hat{b}$ and $\hat{a}$ axis, respectively. As the $k_2$ component develops, the amplitude of the $k_1$ component is reduced, which indicates a 2k non-collinear magnetic structure. Density functional theory is used to calculate the energies of these magnetic structures and to show the $k_1$ phase is a metal so $T_{\mathrm{N1}}$ is a rare example of a unit-cell-preserving second-order phase transition from a paramagnetic semiconductor to an antiferromagnetic metal. DFT indicates the transition at $T_{\mathrm{N2}}$ to a doubled unit cell reduces the carrier density of the metal, which is consistent with resistivity data.

cond-mat.str-el↗

arXiv2023

Fragile superconductivity in a Dirac metal

Studying superconductivity in Dirac semimetals is an important step in understanding quantum matter with topologically non-trivial order parameters. We report on the properties of the superconducting phase in single crystals of the Dirac material LaCuSb2 prepared by the self-flux method. We find that chemical and hydrostatic pressure drastically suppress the superconducting transition. Furthermore, due to large Fermi surface anisotropy, magnetization and muon spin relaxation measurements reveal Type-II superconductivity for applied magnetic fields along the $a$-axis, and Type-I superconductivity for fields along the $c$-axis. Specific heat confirms the bulk nature of the transition, and its deviation from single-gap $s$-wave BCS theory suggests multigap superconductivity. Our tight-binding model points to an anisotropic gap function arising from the spin-orbital texture near the Dirac nodes, providing an explanation for the appearance of an anomaly in specific heat well below $T_c$. Given the existence of superconductivity in a material harboring Dirac fermions, LaCuSb2 proves an interesting material candidate in the search for topological superconductivity.

cond-mat.supr-con↗

arXiv2023

Chemical tuning of a honeycomb magnet through a critical point

BaCo2(AsO4)2 (BCAO) has seen extensive study since its initial identification as a proximate Kitaev quantum spin liquid candidate. Thought to be described by the highly anisotropic XXZ-J_1-J_3 model, the ease with which magnetic order is suppressed in the system indicates proximity to a spin liquid phase. Upon chemical tuning via partial arsenic substitution with vanadium, we show an initial suppression of long-range incommensurate order in the BCAO system to T = 3.0 K, followed by increased spin freezing at higher substitution levels. Between these two regions, at around 10% substitution, the system is shown to pass through a critical point where the competing J_1/J_3 exchange interactions become more balanced, producing a more complex magnetic ground state, likely stabilized by quantum fluctuations. This state shows how slight compositional change in magnetically-frustrated systems may be leveraged to tune ground state degeneracies and potentially realize a quantum spin liquid state.

cond-mat.str-el↗

arXiv2023

An Algorithm for Subtraction of Doublet Emission Lines in Angle-Resolved Photoemission Spectroscopy

Plasma discharge lamps are widely utilized in the practice of angle-resolved photoemission spectroscopy (ARPES) experiments as narrow-linewidth ultraviolet photon sources. However, many emission lines such as Ar-I, Ne-I, and Ne-II have closely spaced doublet emission lines, which result in superimposed replica on the measured ARPES spectra. Here, we present a simple method for subtracting the contribution of these doublet emission lines from photoemission spectra. Benchmarking against ARPES spectra of well-characterized 2D materials, we demonstrate that this algorithm manages to subtract the doublet signal and reproduce the key features of the monochromated He-I$α$ spectra in a physically sound manner that reliably reproduces quantifiable dispersion relations and quasiparticle lifetimes.

physics.ins-det↗

arXiv2023

The Reverse Quantum Limit: Implications for Unconventional Quantum Oscillations in YbB$_{12}$

Beyond the quantum limit, many-body effects are expected to induce unusual electronic phase transitions. Materials possessing metallic ground states with strong interactions between localized and itinerant electronic states are natural candidates for the realization of such quantum phases. However, the electronic correlations responsible for increasing the likelihood of novel phases simultaneously place the quantum limit beyond the reach of laboratory magnets. Here we propose these difficulties can be surmounted in materials with strong correlations and insulating ground states. Strong correlations in insulators and high magnetic fields conspire to fill Landau levels in the reverse order compared to conventional metals, such that the lowest Landau level is the first observed. Consequently, the quantum limit in strongly correlated insulators is reached in reverse and at fields accessible in laboratories. Quantum oscillations measured at high fields in YbB12 are shown to have features consistent with the reverse quantum limit. These include how quantum oscillations move in lock step with the angular evolution of the insulator-metal transition and the field dependence of the quantum oscillation frequency. We argue that close to the insulator-metal transition, the insulating state should be viewed through the lens of a magnetic field-induced electronic instability affecting the lowest Landau level states in the quantum limit.

cond-mat.str-el↗

arXiv2023

Influence of magnetic and electric fields on universal conductance fluctuations in thin films of the Dirac semi-metal Cd3As2

Time-reversal invariance and inversion symmetry are responsible for the topological band structure in Dirac semimetals. These symmetries can be broken by applying an external magnetic or electric field, resulting in fundamental changes to the ground state Hamiltonian and a topological phase transition. We probe these changes via the magnetic-field dependence and gate voltage-dependence of universal conductance fluctuations in top-gated nanowires of the prototypical Dirac semimetal Cd3As2. As the magnetic field is increased beyond the phase-breaking field, we find a factor of sqrt(2) reduction in the magnitude of the universal conductance fluctuations, in agreement with numerical calculations that study the effect of broken time reversal symmetry in a 3D Dirac semimetal. In contrast, the magnitude of the fluctuations increases monotonically as the chemical potential is gated away from the charge neutrality point. This effect cannot be attributed to broken inversion symmetry, but can be explained by Fermi surface anisotropy. The concurrence between experimental data and theory in our study provides unequivocal evidence that universal conductance fluctuations are the dominant source of intrinsic transport fluctuations in mesoscopic Cd3As2 devices and offers a promising general methodology for probing the effects of broken symmetry in topological quantum materials.

cond-mat.mes-hall↗

arXiv2023

Machine-guided Design of Oxidation Resistant Superconductors for Quantum Information Applications

Decoherence in superconducting qubits has long been attributed to two level systems arising from the surfaces and interfaces present in real devices. A recent significant step in reducing decoherence was the replacement of superconducting niobium by superconducting tantalum, resulting in a tripling of transmon qubit lifetimes (T1). One of these surface variables, the identity, thickness, and quality of the native surface oxide, is thought to play a major role as tantalum only has one oxide whereas niobium has several. Here we report the development of a thermodynamic metric to rank materials based on their potential to form a well-defined, thin, surface oxide. We first compute this metric for known binary and ternary metal alloys using data available from Materials Project, and experimentally validate the strengths and limits of this metric through preparation and controlled oxidation of 8 known metal alloys. Then we train a convolutional neural network to predict the value of this metric from atomic composition and atomic properties. This allows us to compute the metric for materials that are not present in materials project, including a large selection of known superconductors, and, when combined with Tc, allow us to identify new candidate superconductors for quantum information science (QISE) applications. We test the oxidation resistance of a pair of these predictions experimentally. Our results are expected to lay the foundation for tailored and rapid selection of improved superconductors for QISE.

cond-mat.supr-con↗

arXiv2022

Closed-loop machine learning for discovery of novel superconductors

The discovery of novel materials drives industrial innovation, although the pace of discovery tends to be slow due to the infrequency of "Eureka!" moments. These moments are typically tangential to the original target of the experimental work: "accidental discoveries". Here we demonstrate the acceleration of intentional materials discovery - targeting material properties of interest while generalizing the search to a large materials space with machine learning (ML) methods. We demonstrate a closed-loop ML discovery process targeting novel superconducting materials, which have industrial applications ranging from quantum computing to sensors to power delivery. By closing the loop, i.e. by experimentally testing the results of the ML-generated superconductivity predictions and feeding data back into the ML model to refine, we demonstrate that success rates for superconductor discovery can be more than doubled. In four closed-loop cycles, we discovered a new superconductor in the Zr-In-Ni system, re-discovered five superconductors unknown in the training datasets, and identified two additional phase diagrams of interest for new superconducting materials. Our work demonstrates the critical role experimental feedback provides in ML-driven discovery, and provides definite evidence that such technologies can accelerate discovery even in the absence of knowledge of the underlying physics.

cond-mat.supr-con↗

arXiv2022

Misfit Layered Compounds: Unique, Tunable Heterostructured Materials with Untapped Properties

Building on discoveries in graphene and two-dimensional (2D) transition metal dichalcogenides, van der Waals (VdW) layered heterostructures - stacks of such 2D materials - are being extensively explored with resulting new discoveries of novel electronic and magnetic properties in the ultrathin limit. Here we review a class of naturally occurring heterostructures - so called misfits - that combine disparate VdW layers with complex stacking. Exhibiting remarkable structural complexity and diversity of phenomena, misfits provide a platform on which to systematically explore the energetics and local bonding constraints of heterostructures and how they can be used to engineer novel quantum fabrics, electronic responsiveness, and magnetic phenomena. Like traditional classes of layered materials, they are often exfoliatable and thus also incorporatable as units in manually or robotically stacked heterostructures. Here we review the known classes of misfit structures, the tools for their single crystal and thin film synthesis, the physical properties they exhibit, and computational and characterization tools that are unraveling their complexity. Directions for future research are also discussed.

cond-mat.mtrl-sci↗

arXiv2022

Single Crystal Growth Tricks and Treats

Single crystal growth is a widely explored method of synthesizing materials in the solid state. The last few decades have seen significant improvements in the techniques used to synthesize single crystals, but there has been comparatively little discussion on ways to disseminate this knowledge. We aim to change that. Here we describe the principles of known single crystal growth techniques as well as lesser-known variations that have assisted in the optimization of defect control in known materials. We offer a perspective on how to think about these synthesis methods in a grand scheme. We consider the temperature interdependence with the reaction time as well as ways to carry out synthesis to scale up and address some outstanding synthesis challenges. We hope our descriptions will aid in technological advancements as well as further developments to gain even better control over synthesis.

cond-mat.mtrl-sci↗

arXiv2022

Magnetic phase crossover in strongly correlated EuMn2P2

Strong electron correlations underlie a plethora of electronic and magnetic components and devices and are often used to identify and probe novel ground states in quantum materials. Herein we report a magnetic phase crossover in EuMn2P2, an insulator which shows Eu antiferromagnetism at TN=17K, but no phase transition attributed to Mn magnetism. The absence of a Mn magnetic phase transition contrasts with the formation of long-range Mn order at T=130K in isoelectronic EuMn2Sb2 and EuMn2As2. Temperature-dependent specific heat and 31P NMR measurements provide evidence for the development of Mn magnetic correlations from T=250-100 K. Density functional theory calculations demonstrate an unusual sensitivity of the band structure to the details of the imposed Mn and Eu magnetic order, with antiferromagnetic Mn order required to recapitulate an insulating state. Our results imply a picture in which long range Mn magnetic order is suppressed by chemical pressure, but that magnetic correlations persist, narrowing bands and producing an insulating state.

cond-mat.str-el↗

arXiv2022

Hydrothermal synthesis of ordered corkite, PbFe3(PO4)(SO4)(OH)6, a S = 5/2 kagomé antiferromagnet

Corkite, PbFe3(PO4)(SO4)(OH)6, an understudied relative of the jarosite family of Heisenberg antiferromagnets, has been synthesized and its magnetic properties characterized for the first time. Relative to natural samples, synthetic corkite displays signatures in both infrared and Raman spectra of a more ordered arrangement of polyanion groups about the kagomé sublattice that retains inversion symmetry. Magnetic susceptibility measurements reveal that dried corkite undergoes a transition to a long-range, antiferromagnetically-ordered state below TN = 48 K, lower than that observed in the majority of jarosite phases, and indicative of further spin frustration. Curie-Weiss fitting of the measured magnetic susceptibility yields an effective magnetic moment of peff = 6.29(1) muB/Fe^3+ and theta_CW = -526.0(1.1) K, analogous to that observed in similar high-spin Fe^3+ systems, and indicative of strong antiferromagnetic coupling. Estimation of the change in magnetic entropy as a function of temperature from T = 0 K to T = 195 K, dS_mag = 14.86 J/mol_Fe^3+ K, is also in good agreement with the dS_mag = Rln(2S+1) = 14.9 J/mol K expected for a S = 5/2 system. In comparison to the pure jarosites, where both structure and magnetism remain largely invariant upon a variety of chemical substitutions, the replacement of one sulfate group per formula unit with a higher-valent phosphate group applies additional steric and electronic pressure on the kagomé lattice in corkite, further frustrating the magnetic ground state of the material. Corkite thus represents both an outlier in the known body of jarosite-type materials, and an illustration of how existing structures may be further strained in the development of highly frustrated magnetic systems.

cond-mat.str-el↗

arXiv2022

Integer quantum Hall effect and enhanced g-factor in quantum confined Cd3As2 films

We investigate the integer quantum Hall effect in Cd3As2 thin films under conditions of strong to moderate quantum confinement (thicknesses of 10 nm, 12 nm, 15 nm). In all the films, we observe the integer quantum Hall effect in the spin-polarized lowest Landau level (filling factor ν = 1) and at spin-degenerate higher index Landau levels with even filling factors (ν = 2,4,6). With increasing quantum confinement, we also observe a lifting of the Landau level spin degeneracy at ν = 3, manifest as the emergence of an anomaly in the longitudinal and Hall resistivity. Tight-binding calculations show that the enhanced g-factor likely arises from a combination of quantum confinement and corrections from nearby subbands. We also comment on the magnetic field induced transition from an insulator to a quantum Hall liquid when the chemical potential is near the charge neutrality point.

cond-mat.mes-hall↗