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Christopher Broyles

Publications and source records attributed to Christopher Broyles.

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Resistive Switching and Neuromorphic Computing in Metal/Nb:SrTiO$_3$: Mechanisms, Interface Physics, and Charge Transport

Resistive switching (RS) in Nb-doped SrTiO$_3$ (Nb:STO) based memristive devices has attracted sustained interest in information processing and novel computing because of its forming-free operation, large on/off ratio, and gradual conductance modulation. Metal/Nb:STO Schottky junctions have emerged as a prototypical system for understanding RS mechanisms. Despite more than two decades of research, the physical origin of RS remains controversial, with proposed mechanisms including charge trapping and detrapping, oxygen vacancy migration, tunneling, interfacial redox reactions, and conductive filament formation. In this review, we examine these seemingly competing mechanisms and show that many experimental observations can be understood within a unified framework centered on the formation and evolution of an extrinsic interfacial layer at the metal/Nb:STO interface. We discuss how interface quality and defect-mediated processes, including proton incorporation, oxygen vacancy dynamics, and tunneling, govern Schottky barrier modulation and RS behavior. We further summarize how fabrication conditions, measurement protocols, and aging influence the interface formation and switching characteristics. This review establishes an integrated picture of M/Nb:STO heterojunctions and provides design principles for reliable oxide memristive devices through interface and defect engineering in M/Nb:STO and M/oxide/Nb:STO systems.

cond-mat.mtrl-sci

Field-rigid Ising antiferromagnetism with giant spin-flip fields in Van der Waals UOTe

Van der Waals antiferromagnets provide a route to thickness-controlled magnetic order, but few combine high-temperature Ising order with conducting, correlated, and topological electronic structure. Here we show that UOTe realizes this combination. Magnetic susceptibility reveals a strongly anisotropic paramagnetic response, while neutron diffraction establishes c-axis antiferromagnetic order below $T_N \simeq 150$ K with an order-parameter exponent $\beta = 0.14$, close to the two-dimensional Ising value. Torque magnetometry further shows that the ordered state remains well described by a uniaxial antiferromagnet below the high-field transition. Pulsed-field magnetization up to 73 T shows that the ordered state survives to very large fields applied along the c axis before entering a broad metamagnetic regime that begins near 50 T, and remains unsaturated at the highest measured field. Angle-dependent proximity detector oscillator measurements show that the metamagnetic instability is set by the field component along the ordered moment direction, providing direct evidence for Ising-like field rigidity. UOTe therefore establishes a field-rigid Ising antiferromagnet with giant spin-flip fields in a compensated Van der Waals metal, where high-temperature c-axis order, quasi-two-dimensional magnetic criticality, Kondo-associated uranium 5f hybridization, metallic transport, and symmetry-enabled topology coexist in a single material.

cond-mat.str-el

Layer-dependent antiferromagnetic Chern and axion insulating states in UOTe

Magnetic topological insulators have received significant interest due to their dissipationless edge states, which promise advances in energy-efficient electronic transport. However, the magnetic topological insulator state has typically been found in ferromagnets (FMs) that suffer from low magnetic ordering temperatures and stray fields. Identifying an antiferromagnetic topological insulator that exhibits the quantum anomalous Hall effect (QAHE) with a relatively high N\'eel temperature has been a longstanding challenge. Here, we focus on the recently discovered van der Waals (vdW) antiferromagnet (AFM) UOTe, which not only features a high N\'eel temperature (\(\sim\)150K) but also exhibits intriguing Kondo interaction and topological characteristics. Our systematic analysis of the layer-dependent topological phases based on \textit{ab} initio computations predicts the two-layer UOTe film to be an ideal 2D AFM Chern insulator in which the Hall conductivity is quantized with a fully compensated spin magnetization. By applying an in-plane strain or electric field, we show how the itinerancy of U-5f electrons can be manipulated to trigger a transition between the nontrivial ($C = 1$) and trivial ($C = 0$) phases. Interestingly, the 3-layer UOTe film is found to have zero charge conductance but it hosts a quantized spin Hall conductivity (SHC) with finite magneto-electric coupling, suggesting the presence of an axion insulator-like state. The unique magnetic structure of UOTe supports a layer-tunable topology in which films with an odd number of layers are axion-like insulators, while films with an even number of layers are Chern insulators, and the bulk material is a Dirac semimetal. Our study offers a new intrinsic AFM materials platform for realizing correlated topological phases for next-generation spintronics applications and fundamental science studies.

cond-mat.mtrl-sci

Odd-Parity Quasiparticle Interference in the Superconductive Surface State of UTe2

Although no known material exhibits intrinsic topological superconductivity, wherein spin-triplet odd-parity electron pairing occurs, UTe2 is now the leading representative of this class. Conventionally, the parity of the superconducting order parameter may be established by using Bogoliubov quasiparticle interference (QPI) imaging. However, odd-parity superconductors should support a topological quasiparticle surface band (QSB) at energies within the maximum superconducting energy gap. QPI would then be dominated by the electronic structure of the QSB and only reveal the characteristics of the bulk order parameter excursively. Here, we visualize quasiparticle interference patterns of UTe2 and find that, at the (0-11) cleave surface, a new band of Bogoliubov quasiparticles appears only in the superconducting state. QPI visualization then allows study of dispersion of states within this QSB, which we demonstrate exists only within the range of Fermi momenta projected onto the (0-11) surface. Finally, we develop a theoretical framework to predict the QPI signatures of such a QSB at the (0-11) surface of UTe2. Its predictions are most consistent with the experimental results if the bulk superconducting gap function exhibits time-reversal conserving, odd-parity, a-axis nodal, B3u symmetry.

cond-mat.supr-con

High temperature surface state in Kondo insulator U$_3$Bi$_4$Ni$_3$

The resurgence of interest in Kondo insulators has been driven by two major mysteries: the presence of metallic surface states and the observation of quantum oscillations. To further explore these mysteries, it is crucial to investigate another similar system beyond the two existing ones, SmB$_6$ and YbB$_{12}$. Here, we address this by reporting on a Kondo insulator, U$_3$Bi$_4$Ni$_3$. Our transport measurements reveal that a surface state emerges below 250 K and dominates transport properties below 150 K, which is well above the temperature scale of SmB$_6$ and YbB$_{12}$. At low temperatures, the surface conductivity is about one order of magnitude higher than the bulk. The robustness of the surface state indicates that it is inherently protected. The similarities and differences between U$_3$Bi$_4$Ni$_3$ and the other two Kondo insulators will provide valuable insights into the nature of metallic surface states in Kondo insulators and their interplay with strong electron correlations.

cond-mat.str-el

Pair Wavefunction Symmetry in UTe2 from Zero-Energy Surface State Visualization

Although nodal spin-triplet topological superconductivity appears probable in UTe2, its superconductive order-parameter $\Delta_k$ remains unestablished. In theory, a distinctive identifier would be the existence of a superconductive topological surface band (TSB), which could facilitate zero-energy Andreev tunneling to an s-wave superconductor, and also distinguish a chiral from non-chiral $\Delta_k$ via enhanced s-wave proximity. Here we employ s-wave superconductive scan-tips and detect intense zero-energy Andreev conductance at the UTe2 (0-11) termination surface. Imaging reveals sub-gap quasiparticle scattering interference signatures with a-axis orientation. The observed zero-energy Andreev peak splitting with enhanced s-wave proximity, signifies that $\Delta_k$ of UTe2 is a non-chiral state: B1u, B2u or B3u. However, if the quasiparticle scattering along the a-axis is internodal, then a non-chiral B3u state is the most consistent for UTe2.

cond-mat.supr-con

UOTe: Kondo-interacting topological antiferromagnet in a van der Waals lattice

Since the initial discovery of two-dimensional van der Waals (vdW) materials, significant effort has been made to incorporate the three properties of magnetism, band structure topology, and strong electron correlations $-$ to leverage emergent quantum phenomena and expand their potential applications. However, the discovery of a single vdW material that intrinsically hosts all three ingredients has remained an outstanding challenge. Here we report the discovery of a Kondo-interacting topological antiferromagnet in the vdW 5$f$ electron system UOTe. It has a high antiferromagnetic (AFM) transition temperature of 150 K, with a unique AFM configuration that breaks the combined parity and time reversal ($PT$) symmetry in an even number of layers while maintaining zero net magnetic moment. Our angle-resolved photoemission spectroscopy (ARPES) measurements reveal Dirac bands near the Fermi level, which combined with our theoretical calculations demonstrate UOTe as an AFM Dirac semimetal. Within the AFM order, we observed the presence of the Kondo interaction, as evidenced by the emergence of a 5$f$ flat band near the Fermi level below 100 K and hybridization between the Kondo band and the Dirac band. Our density functional theory calculations in its bilayer form predict UOTe as a rare example of a fully-compensated AFM Chern insulator.

cond-mat.str-el

Observation of vortex stripes in UTe$_2$

Quantum vortices are fundamentally important for properties of superconductors. In conventional type-II superconductor they determine the magnetic response of the system and tend to form regular lattices. UTe$_2$ is a recently discovered heavy fermion superconductor exhibiting many anomalous macroscopic behaviors. However, the question whether it has a multicomponent order parameter remains open. Here, we study magnetic properties of UTe$_2$ by employing scanning superconducting quantum interference device microscopy. We find vortex behavior which is very different from that in ordinary superconductors. We imaged vortices generated by cooling in magnetic field applied along different crystalline directions. While a small out-of-plane magnetic field produces typical isolated vortices, higher field generates vortex stripe patterns which evolve with vortex density. The stripes form at different locations and along different directions in the surface plane when the vortices are crystalized along the crystalline b or c axes. The behavior is reproduced by our simulation based on an anisotropic two-component order parameter. This study shows that UTe$_2$ has a nontrivial disparity of multiple length scales, placing constraints on multicomponent superconductivity. The tendency of vortex stripe formation and their control by external field may be useful in fluxonics applications.

cond-mat.supr-con

Structure-Driven Prediction of Magnetic Order in Uranium Compounds

The advancement of machine learning technologies has revolutionized the search and optimization of material properties. These algorithms often rely on theoretical calculations, such as density functional theory (DFT), for data inputs and validation, which are not always effective for uranium-based materials due to their strong electron correlations. This study presents a computationally inexpensive machine learning approach, specifically a random forest classifier, to predict the magnetic ground states of uranium compounds using only structural inputs. Our model, trained on a curated dataset of experimentally-verified magnetic orders, achieves a mean accuracy of 60.2%, significantly outperforming random chance. By excluding computationally intensive DFT calculations, our method offers a faster and reliable alternative for discovering new materials with desirable magnetic properties, addressing the challenges posed by strong correlations in quantum materials.

cond-mat.mtrl-sci

A single crystal study of Kagome metals U$_2$Mn$_3$Ge and U$_2$Fe$_3$Ge

Single crystals of U$_2$Mn$_3$Ge and and U$_2$Fe$_3$Ge with a Kagome lattice structure were synthesized using a high-temperature self-flux crystal growth method. The physical properties of these crystals were characterized through measurements of resistivity, magnetism, and specific heat. U$_2$Fe$_3$Ge exhibits ferromagnetic ground state and Anomalous Hall Effect, and U$_2$Mn$_3$Ge demonstrates a complex magnetic structure. Both compounds exhibit large Sommerfeld coefficient, indicating coexistence of heavy Fermion behavior with magnetism. Our results suggest that this U$_2$TM$_3$Ge (TM = Mn, Fe, Co) family is a promising platform to investigate the interplay of magnetism, Kondo physics and the Kagome lattice.

cond-mat.str-el

Tunable Giant Anomalous Hall in a Kondo Lattice Ferromagnet UBiTe

Kondo lattice systems are recognized for potentially hosting a variety of rich topological phases. Several pioneering studies have demonstrated significant anomalous Hall and anomalous Nernst effects in these systems, attributed to the Berry curvature of the hybridization bands. In this study, we investigate UBiTe, a ferromagnetic Kondo lattice system. Our findings reveal that the intrinsic contribution to the anomalous Hall conductivity is closely tied to the Kondo coherence temperature. Moreover, we demonstrate that slight shifts in the Fermi level across three different samples significantly influence this intrinsic contribution, in alignment with the Berry curvature localized within the narrow hybridization bands. This provides a stark contrast to the less pronounced sensitivity observed in weakly correlated Weyl semimetals, underscoring the distinctive electronic properties of Kondo lattice systems. The anomalous Hall conductivity of one samples ranks among the highest reported for topological magnetic materials.

cond-mat.str-el

Quantum Oscillations in kagome metals CsTi3Bi5 and RbTi3Bi5

We report quantum oscillation measurements on the kagome compounds ATi$_3$Bi$_5$ (A=Rb, Cs) in magnetic fields up to 41.5 T and temperatures down to 350 mK. In addition to the frequencies observed in previous studies, we have observed multiple unreported frequencies above 2000 T in CsTi$_3$Bi$_5$ using a tunnel diode oscillator technique. We compare these results against density functional theory calculations and find good agreement with the calculations in the number of peaks observed, frequency, and the dimensionality of the Fermi surface. For RbTi$_3$Bi$_5$ we have obtained a different quantum oscillation spectrum, although calculated quantum oscillation frequencies for the Rb compound are remarkably similar to the Cs compound, calling for further studies.

cond-mat.str-el

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 principal 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 detected experimentally. Here 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.

cond-mat.str-el

Breakdown of the scaling relation of anomalous Hall effect in Kondo lattice ferromagnet USbTe

The interaction between strong correlation and Berry curvature is an open territory of in the field of quantum materials. Here we report large anomalous Hall conductivity in a Kondo lattice ferromagnet USbTe which is dominated by intrinsic Berry curvature at low temperatures. However, the Berry curvature induced anomalous Hall effect does not follow the scaling relation derived from Fermi liquid theory. The onset of the Berry curvature contribution coincides with the Kondo coherent temperature. Combined with ARPES measurement and DMFT calculations, this strongly indicates that Berry curvature is hosted by the flat bands induced by Kondo hybridization at the Fermi level. Our results demonstrate that the Kondo coherence of the flat bands has a dramatic influence on the low temperature physical properties associated with the Berry curvature, calling for new theories of scaling relations of anomalous Hall effect to account for the interaction between strong correlation and Berry curvature.

cond-mat.str-el

Tuning the parity of superconductivity in CeRh2As2 via pressure

In the recently discovered heavy fermion superconductor CeRh2As2, a magnetic field induced phase transition has been observed inside the superconducting state, which is proposed to be a transition from an even to an odd-parity superconducting state. The odd-parity superconducting state and its large upper critical field has been explained by local inversion symmetry breaking and consequent Rashba spin-orbit coupling. Here we report the experimental tuning of the parity of superconductivity in CeRh2As2 via applied pressure. Superconductivity is enhanced by pressure after its initial suppression, forming a second dome. However, the odd-parity state only exists in the first dome and the second dome is dominated by the even-parity state. This parity switch of superconductivity under pressure is consistent with the competition between Rashba spin-orbit coupling and interlayer hopping in determining the parity of superconductivity in systems with local inversion symmetry breaking. Our results provide insightful guidance on how to look for new odd-parity superconductors.

cond-mat.supr-con

Detection of a Pair Density Wave State in UTe$_2$

Spin-triplet topological superconductors should exhibit many unprecedented electronic properties including fractionalized electronic states relevant to quantum information processing. Although UTe$_2$ may embody such bulk topological superconductivity, its superconductive order-parameter $\Delta(\mathbf{k})$ remains unknown. Many diverse forms for $\Delta(\mathbf{k})$ are physically possible in such heavy fermion materials. Moreover, intertwined density waves of spin (SDW), charge (CDW) and pairs (PDW) may interpose, with the latter state exhibiting spatially modulating superconductive order-parameter $\Delta(\mathbf{r})$, electron pair density and pairing energy-gap. Hence, the newly discovered CDW state in UTe$_2$ motivates the prospect that a PDW state may exist in this material. To search for it, we visualize the pairing energy-gap with $\mu$$eV$-scale energy-resolution using superconductive STM tips. We detect three PDWs, each with peak-peak gap modulations circa 10 $\mu$$eV$ and at incommensurate wavevectors $\mathbf{P}_{i=1,2,3}$ that are indistinguishable from the wavevectors $\mathbf{Q}_{i=1,2,3}$ of the prevenient CDW. Concurrent visualization of the UTe$_2$ superconductive PDWs and the non-superconductive CDWs reveals that every $\mathbf{P}_i$ : $\mathbf{Q}_i$ pair exhibits a relative phase $\delta\phi \approx \pi$. From these observations, and given UTe$_2$ as a spin-triplet superconductor, this PDW state should be a spin-triplet pair density wave. While such states do exist in superfluid $^{3}$He, for superconductors they are unprecedented.

cond-mat.supr-con

The effect of the interlayer ordering on the Fermi surface of Kagome superconductor CsV$_3$Sb$_5$ revealed by quantum oscillations

The connection between unconventional superconductivity and charge density waves (CDW) has intrigued the condensed matter community and found much interest in the recently discovered superconducting Kagome family of AV$_3$Sb$_5$ (A = K, Cs, Rb). Xray diffraction and Raman spectroscopy measurements established that the CDW order in CsV$_3$Sb$_5$ comprises of a 2x2x4 structure with stacking of layers of star-of-David (SD) and inverse-star-of-David (ISD) pattern along the $c$-axis direction. Such interlayer ordering will induce a vast normalization of the electronic ground state; however, it has not been observed in Fermi surface measurements. Here we report quantum oscillations of CsV$_3$Sb$_5$ using tunnel diode oscillator frequency measurements. We observed a large number of frequencies, many of which were not reported. The number of frequencies can not be explained by DFT calculations when only SD or ISD distortion is considered. Instead, our results are consistent with calculations when interlayer ordering is taken into account, providing strong evidence that CDW phase of CsV$_3$Sb$_5$ has complicated structure distortion which in turn has dramatic effects on the Fermi surface properties.

cond-mat.str-el