arXiv subjects

Chris Leighton

Publications and source records attributed to Chris Leighton.

At least 19 recordsLinked to original sources

arXiv2026

Anomalous Compressibility and Electronic Robustness of Metallic Delafossite PdCoO$_2$ under Pressure

The layered delafossite PdCoO$_2$ is an exceptional oxide metal whose ultrahigh conductivity arises from a Pd-derived nearly-free-electron band. Here, high-pressure single-crystal X-ray diffraction combined with first-principles calculations is used to investigate its structural, bonding, and electronic evolution up to 10 GPa. PdCoO$_2$ retains the rhombohedral R-3m structure throughout the investigated pressure range, with no structural phase transition. The lattice exhibits an unusual anisotropic compression, with the in-plane a-axis contracting more strongly than the stacking c-axis, opposite to the behavior of most layered materials. Despite this anomalous compressibility, only minor changes are observed in the local Pd-O and Co-O coordination environments, indicating a remarkably rigid bonding framework. Crystal orbital Hamilton population analysis reveals only subtle strengthening of the existing bonding interactions, without the emergence of destabilizing Pd-related antibonding states. Consistent with these findings, the Pd-derived metallic band and quasi-two-dimensional Fermi surface remain essentially unchanged under compression. Boltzmann transport calculations further show that the in-plane conductivity is nearly pressure-independent, whereas the out-of-plane conductivity decreases modestly, resulting in a slight increase in transport anisotropy. These results demonstrate that the anomalous compressibility of PdCoO$_2$ originates from its robust chemical bonding network, which preserves both the crystal structure and the highly conductive Pd-derived metallic state under pressure.

cond-mat.mtrl-sci↗

arXiv2026

Mechanically Exfoliated Metallic Delafossite PdCoO2 Nanomembranes: Quantum Transport and Electrical Evaluation Toward Interconnect Applications

Metallic delafossite oxides have drawn attention for their ultralow resistivity and coherent electronic transport. However, mesoscopic transport studies are hindered by the limited access to high quality nanoscale devices. Here, we report single crystalline PdCoO2 nanomembranes, enabling exploration of quasi two dimensional (2D) transport. Shubnikov de Haas and Aharonov Bohm oscillations under different magnetic field orientations are observed at low temperatures, from which the electron effective mass and electron phase coherence length are extracted. Beyond quantum transport, the electrical performance of PdCoO2 toward interconnect applications is evaluated. A nearly thickness independent room temperature resistivity is observed for flakes down to 40 nm thickness. The nanomembranes exhibit a breakdown current density up to 113 MA cm-2, with excellent thermal stability and electromigration resistance. These results demonstrate that mechanically exfoliated PdCoO2 flakes preserve the high crystalline and electronic quality of bulk crystals in the quasi-2D limit, providing a useful platform for mesoscopic transport studies and interconnect applications.

cond-mat.mes-hall↗

arXiv2025

Sub-tesla on-chip nanomagnetic metamaterial platform for angle-resolved photoemission spectroscopy

Magnetically controlled states in quantum materials are central to their unique electronic and magnetic properties. However, direct momentum-resolved visualization of these states via angle-resolved photoemission spectroscopy (ARPES) has been hindered by the disruptive effect of magnetic fields on photoelectron trajectories. Here, we introduce an \textit{in-situ} method that is, in principle, capable of applying magnetic fields up to 1 T. This method uses substrates composed of nanomagnetic metamaterial arrays with alternating polarity. Such substrates can generate strong, homogeneous, and spatially confined fields applicable to samples with thicknesses up to the micron scale, enabling ARPES measurements under magnetic fields with minimal photoelectron trajectory distortion. We demonstrate this minimal distortion with ARPES data taken on monolayer graphene. Our method paves the way for probing magnetic field-dependent electronic structures and studying field-tunable quantum phases with state-of-the-art energy-momentum resolutions.

cond-mat.mes-hall↗

arXiv2025

Dual Optical Hyperbolicity of PdCoO$_2$ and PdCrO$_2$ Delafossite Single Crystals

Hyperbolic materials exhibit a very peculiar optical anisotropy with simultaneously different signs of the dielectric tensor components. This anisotropy allows the propagation of exotic surface-wave excitations like hyperbolic phonons and plasmon polaritons. While hyperbolic materials hold promise for applications in subwavelength photonics and enhanced light-matter interactions, their natural occurrence is limited to few materials, often accompanied by significant dielectric losses and limited hyperbolic spectral bandwidth. Focusing on PdCoO$_2$ and PdCrO$_2$ delafossite transition-metal oxides, in this paper we demonstrate their unique dual hyperbolic regimes: one localized around a phonon absorption in the mid-infrared spectral region, and the other extending into the visible range. Both hyperbolic regimes show exceptional properties including low dissipation and high hyperbolic quality factors. These results pave the way for innovative applications of delafossite layered metals in subwavelength photonics, imaging, and sensing.

cond-mat.mtrl-sci↗

arXiv2023

Crystal-Chemical Origins of the Ultrahigh Conductivity of Metallic Delafossites

Despite their highly anisotropic complex-oxidic nature, certain delafossite compounds (e.g., PdCoO2, PtCoO2) are the most conductive oxides known, for reasons that remain poorly understood. Their room-temperature conductivity can exceed that of Au, while their low-temperature electronic mean-free-paths reach an astonishing 20 microns. It is widely accepted that these materials must be ultrapure to achieve this, although the methods for their growth (which produce only small crystals) are not typically capable of such. Here, we first report a new approach to PdCoO2 crystal growth, using chemical vapor transport methods to achieve order-of-magnitude gains in size, the highest structural qualities yet reported, and record residual resistivity ratios (>440). Nevertheless, the first detailed mass spectrometry measurements on these materials reveal that they are not ultrapure, typically harboring 100s-of-parts-per-million impurity levels. Through quantitative crystal-chemical analyses, we resolve this apparent dichotomy, showing that the vast majority of impurities are forced to reside in the Co-O octahedral layers, leaving the conductive Pd sheets highly pure (~1 ppm impurity concentrations). These purities are shown to be in quantitative agreement with measured residual resistivities. We thus conclude that a previously unconsidered "sublattice purification" mechanism is essential to the ultrahigh low-temperature conductivity and mean-free-path of metallic delafossites.

cond-mat.mtrl-sci↗

arXiv2023

Topological Kinetic Crossover in a Nanomagnet Array

Ergodic kinetics, which are critical to equilibrium thermodynamics, can be constrained by a system's topology. We study a model nanomagnetic array in which such constraints visibly affect the behavior. In this system, magnetic excitations connect into thermally active one-dimensional strings whose motion can be imaged in real time. At high temperatures, we observe the merging, breaking, and reconnecting of strings, resulting in the system transitioning between topologically distinct configurations. Below a crossover temperature, the string motion is dominated by simple changes in length and shape. In this low temperature regime, the system is energetically stable because of its inability to explore all possible topological configurations. This kinetic crossover suggests a generalizable conception of topologically broken ergodicity and limited equilibration.

cond-mat.mes-hall↗

arXiv2023

Wide-range continuous tuning of the thermal conductivity of $\rm La_{0.5}Sr_{0.5}CoO_{3-δ}$ films via room-temperature ion-gel gating

Solid-state control of the thermal conductivity of materials is of exceptional interest for novel devices such as thermal diodes and switches. Here, we demonstrate the ability to continuously tune the thermal conductivity of nanoscale films of $\rm La_{0.5}Sr_{0.5}CoO_{3-δ}$ (LSCO) by a factor of over 5, via a room-temperature electrolyte-gate-induced non-volatile topotactic phase transformation from perovskite (with $δ\approx 0.1$) to an oxygen-vacancy-ordered brownmillerite phase (with $δ=0.5$), accompanied by a metal-insulator transition. Combining time-domain thermoreflectance and electronic transport measurements, model analyses based on molecular dynamics and Boltzmann transport, and structural characterization by X-ray diffraction, we uncover and deconvolve the effects of these transitions on heat carriers, including electrons and lattice vibrations. The wide-range continuous tunability of LSCO thermal conductivity enabled by low-voltage (below 4 V) room-temperature electrolyte gating opens the door to non-volatile dynamic control of thermal transport in perovskite-based functional materials, for thermal regulation and management in device applications.

cond-mat.mtrl-sci↗

arXiv2022

Room-Temperature Valence Transition in a Strain-Tuned Perovskite Oxide

Cobalt oxides have long been understood to display intriguing phenomena known as spin-state crossovers, where the cobalt ion spin changes vs. temperature, pressure, etc. A very different situation was recently uncovered in praseodymium-containing cobalt oxides, where a first-order coupled spin-state/structural/metal-insulator transition occurs, driven by a remarkable praseodymium valence transition. Such valence transitions, particularly when triggering spin-state and metal-insulator transitions, offer highly appealing functionality, but have thus far been confined to cryogenic temperatures in bulk materials (e.g., 90 K in Pr1-xCaxCoO3). Here, we show that in thin films of the complex perovskite (Pr1-yYy)1-xCaxCoO3-δ, heteroepitaxial strain tuning enables stabilization of valence-driven spin-state/structural/metal-insulator transitions to at least 291 K, i.e., around room temperature. The technological implications of this result are accompanied by fundamental prospects, as complete strain control of the electronic ground state is demonstrated, from ferromagnetic metal under tension to nonmagnetic insulator under compression, thereby exposing a potential novel quantum critical point.

cond-mat.mtrl-sci↗

arXiv2022

Entropy-driven order in an array of nanomagnets

Long-range ordering is typically associated with a decrease in entropy. Yet, it can also be driven by increasing entropy in certain special cases. We demonstrate that artificial spin ice arrays of single-domain nanomagnets can be designed to produce entropy-driven order. We focus on the tetris artificial spin ice structure, a highly frustrated array geometry with a zero-point Pauli entropy, which is formed by selectively creating regular vacancies on the canonical square ice lattice. We probe thermally active tetris artificial spin ice both experimentally and through simulations, measuring the magnetic moments of the individual nanomagnets. We find two-dimensional magnetic ordering in one subset of these moments, which we demonstrate to be induced by disorder (i.e., increased entropy) in another subset of the moments. In contrast with other entropy-driven systems, the discrete degrees of freedom in tetris artificial spin ice are binary and are both designable and directly observable at the microscale, and the entropy of the system is precisely calculable in simulations. This example, in which the system's interactions and ground state entropy are well-defined, expands the experimental landscape for the study of entropy-driven ordering.

cond-mat.mes-hall↗

arXiv2022

Electrochemically-driven insulator-metal transition in ionic-liquid-gated antiferromagnetic Mott-insulating NiS$_2$ single crystals

Motivated by the existence of superconductivity in pyrite-structure CuS$_2$, we explore the possibility of ionic-liquid-gating-induced superconductivity in the proximal antiferromagnetic Mott insulator NiS$_2$. A clear gating-induced transition from a two-dimensional insulating state to a three-dimensional metallic state is observed at positive gate bias on single crystal surfaces. No evidence for superconductivity is observed down to the lowest measured temperature of 0.45 K, however. Based on transport, energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, atomic force microscopy, and other techniques, we deduce an electrochemical gating mechanism involving a substantial decrease in the S:Ni ratio (over hundreds of nm), which is both non-volatile and irreversible. This is in striking contrast to the reversible, volatile, surface-limited, electrostatic gate effect in pyrite FeS$_2$. We attribute this stark difference in electrochemical vs. electrostatic gating response in NiS$_2$ and FeS$_2$ to the much larger S diffusion coefficient in NiS$_2$, analogous to the different behaviors observed among electrolyte-gated oxides with differing O-vacancy diffusivities. The gating irreversibility, on the other hand, is associated with the lack of atmospheric S; this is in contrast to the better understood oxide case, where electrolysis of atmospheric H$_2$O provides an O reservoir. This study of NiS$_2$ thus provides new insight into electrolyte gating mechanisms in functional materials, in a previously unexplored limit.

cond-mat.mtrl-sci↗

arXiv2021

String Phase in an Artificial Spin Ice

One-dimensional strings of local excitations are a fascinating feature of the physical behavior of strongly correlated topological quantum matter. Here we study strings of local excitations in a classical system of interacting nanomagnets, the Santa Fe Ice geometry of artificial spin ice. We measured the moment configuration of the nanomagnets, both after annealing near the ferromagnetic Curie point and in a thermally dynamic state. While the Santa Fe Ice lattice structure is complex, we demonstrate that its disordered magnetic state is naturally described within a framework of emergent strings. We show experimentally that the string length follows a simple Boltzmann distribution with an energy scale that is associated with the system's magnetic interactions and is consistent with theoretical predictions. The results demonstrate that string description and associated topological characteristics are not unique to quantum models but can also provide a simplifying description of complex classical systems with non-trivial frustration.

cond-mat.mes-hall↗

arXiv2021

Understanding Magnetic Phase Coexistence in Ru$_2$Mn$_{1-x}$Fe$_x$Sn Heusler Alloys: A Neutron Scattering, Thermodynamic, and Phenomenological Analysis

The random substitutional solid solution between the antiferromagnetic (AFM) full-Heusler alloy Ru$_2$MnSn and the ferromagnetic (FM) full-Heusler alloy Ru$_2$FeSn provides a rare opportunity to study FM-AFM phase competition in a near-lattice-matched, cubic system, with full solubility. At intermediate $x$ in Ru$_2$Mn$_{1-x}$Fe$_x$Sn this system displays suppressed magnetic ordering temperatures, spatially coexisting FM and AFM order, and strong coercivity enhancement, despite rigorous chemical homogeneity. Here, we construct the most detailed temperature- and $x$-dependent understanding of the magnetic phase competition and coexistence in this system to date, combining wide-temperature-range neutron diffraction and small-angle neutron scattering with magnetometry and specific heat measurements on thoroughly characterized polycrystals. A complete magnetic phase diagram is generated, showing FM-AFM coexistence between $x \approx 0.30$ and $x \approx 0.70$. Important new insight is gained from the extracted length scales for magnetic phase coexistence (25-100 nm), the relative magnetic volume fractions and ordering temperatures, in addition to remarkable $x$-dependent trends in magnetic and electronic contributions to specific heat. An unusual feature in the magnetic phase diagram (an intermediate FM phase) is also shown to arise from an extrinsic effect related to a minor Ru-rich secondary phase. The established magnetic phase diagram is then discussed with the aid of phenomenological modeling, clarifying the nature of the mesoscale phase coexistence with respect to the understanding of disordered Heisenberg models.

cond-mat.str-el↗

arXiv2019

Soft X-ray Absorption Spectroscopy and Magnetic Circular Dichroism as Operando Probes of Complex Oxide Electrolyte Gate Transistors

Electrolyte-based transistors utilizing ionic liquids/gels have been highly successful in the study of charge-density-controlled phenomena, particularly in oxides. Experimental probes beyond transport have played a significant role, despite challenges to their application in electric double-layer transistors. Here, we demonstrate application of synchrotron soft X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) as operando probes of the charge state and magnetism in ion-gel-gated ferromagnetic perovskite films. Electrochemical response via oxygen vacancies at positive gate bias in LaAlO$_3$(001)/La$_{0.5}$Sr$_{0.5}$CoO$_{3-δ}$ is used as a test case. XAS/XMCD measurements of 4-25 unit-cell-thick films first probe the evolution of hole doping (from the O K-edge pre-peak) and ferromagnetism (at the Co L-edges), to establish a baseline. Operando soft XAS/XMCD of electrolyte-gated films is then demonstrated, using optimized spin-coated gels with thickness $\sim$1 $μ$m, and specific composition. Application of gate voltages up to +4 V is shown to dramatically suppress the O $K$-edge XAS pre-peak intensity and Co $L$-edge XMCD, thus enabling the Co valence and ferromagnetism to be tracked upon gate-induced reduction. Soft XAS and XMCD, with appropriate electrolyte design, are thus established as viable for the operando characterization of electrolyte-gated oxides.

cond-mat.mtrl-sci↗

arXiv2019

Understanding Thermal Annealing of Artificial Spin Ice

We have performed a detailed study of thermal annealing of the moment configuration in artificial spin ice. Permalloy (Ni$_{80}$Fe$_{20}$) artificial spin ice samples were examined in the prototypical square ice geometry, studying annealing as a function of island thickness, island shape, and annealing temperature and duration. We also measured the Curie temperature as a function of film thickness, finding that thickness has a strong effect on the Curie temperature in regimes of relevance to many studies of the dynamics of artificial spin ice systems. Increasing the interaction energy between island moments and reducing the energy barrier to flipping the island moments allows the system to more closely approach the collective low energy state of the moments upon annealing, suggesting new channels for understanding the thermalization processes in these important model systems.

cond-mat.mes-hall↗

arXiv2018

Universal superconducting precursor in perovskite-based oxides

A pivotal challenge posed by unconventional superconductors is to unravel how superconductivity emerges upon cooling from the generally complex normal state. Some of the most prominent unconventional superconductors are oxides: strontium titanate, strontium ruthenate, and the cuprates exhibit greatly different superconducting transition temperatures $T_c$, and although their respective superconducting pairing mechanisms remain unknown, they are thought to differ as well. Here we use nonlinear magnetic response, a probe that is uniquely sensitive to the superconducting precursor, to uncover remarkable universal behavior in these three distinct classes of superconductors. We find unusual exponential temperature dependence of the diamagnetic response above the transition temperature $T_c$, with a characteristic temperature scale that strongly varies with $T_c$. We correlate this scale with the sensitivity of $T_c$ to local stress, and show that it is influenced by intentionally-induced structural disorder. The universal behavior is therefore caused by intrinsic, self-organized structural inhomogeneity, inherent to the oxides perovskite-based structure. The prevalence of such inhomogeneity has far-reaching implications for the interpretation of electronic properties of perovskite-related oxides in general.

cond-mat.supr-con↗

arXiv2018

Giant Electrostatic Modification of Magnetism via Electrolyte-Gate-Induced Cluster Percolation in La$_{1-x}$Sr$_x$CoO$_{3-δ}$

Electrical control of magnetism is a long-standing goal in physics and technology, recently developed electrolyte gating techniques providing a promising route to realization. Validating a recent theoretical prediction, here we demonstrate large enhancement of electrostatic modulation of ferromagnetic order in ion-gel-gated ultrathin La$_{0.5}$Sr$_{0.5}$CoO$_{3-δ}$ by thickness-tuning to the brink of a magnetic percolation transition. Application of only 3-4 V then drives a transition from a short-range-ordered insulator to a robust long-range ferromagnetic metal, realizing giant electrostatic Curie temperature modulation over a 150 K window. In operando polarized neutron reflectometry confirms gate-controlled ferromagnetism, also demonstrating unusually deep penetration of induced magnetization, in further agreement with theory.

cond-mat.str-el↗

arXiv2017

Interface-Induced Phenomena in Magnetism

This article reviews static and dynamic interfacial effects in magnetism, focusing on interfacially-driven magnetic effects and phenomena associated with spin-orbit coupling and intrinsic symmetry breaking at interfaces. It provides a historical background and literature survey, but focuses on recent progress, identifying the most exciting new scientific results and pointing to promising future research directions. It starts with an introduction and overview of how basic magnetic properties are affected by interfaces, then turns to a discussion of charge and spin transport through and near interfaces and how these can be used to control the properties of the magnetic layer. Important concepts include spin accumulation, spin currents, spin transfer torque, and spin pumping. An overview is provided to the current state of knowledge and existing review literature on interfacial effects such as exchange bias, exchange spring magnets, spin Hall effect, oxide heterostructures, and topological insulators. The article highlights recent discoveries of interface-induced magnetism and non-collinear spin textures, non-linear dynamics including spin torque transfer and magnetization reversal induced by interfaces, and interfacial effects in ultrafast magnetization processes.

cond-mat.mtrl-sci↗

arXiv2017

Understanding magnetotransport signatures in networks of connected permalloy nanowires

The change in electrical resistance associated with the application of an external magnetic field is known as the magnetoresistance (MR). The measured MR is quite complex in the class of connected networks of single-domain ferromagnetic nanowires, known as "artificial spin ice", due to the geometrically-induced collective behavior of the nanowire moments. We have conducted a thorough experimental study of the MR of a connected honeycomb artificial spin ice, and we present a simulation methodology for understanding the detailed behavior of this complex correlated magnetic system. Our results demonstrate that the behavior, even at low magnetic fields, can be well-described only by including significant contributions from the vertices at which the legs meet, opening the door to new geometrically-induced MR phenomena.

cond-mat.mes-hall↗