arXiv subjects

C. Leighton

Publications and source records attributed to C. Leighton.

At least 19 recordsLinked to original sources

arXiv2023

Deconstructing Magnetization Noise: Degeneracies, Phases, and Mobile Fractionalized Excitations in Tetris Artificial Spin Ice

Direct detection of spontaneous spin fluctuations, or "magnetization noise", is emerging as a powerful means of revealing and studying magnetic excitations in both natural and artificial frustrated magnets. Depending on the lattice and nature of the frustration, these excitations can often be described as fractionalized quasiparticles possessing an effective magnetic charge. Here, by combining ultrasensitive optical detection of thermodynamic magnetization noise with Monte Carlo simulations, we reveal emergent regimes of magnetic excitations in artificial "tetris ice". A marked increase of the intrinsic noise at certain applied magnetic fields heralds the spontaneous proliferation of fractionalized excitations, which can diffuse independently, without cost in energy, along specific quasi-1D spin chains in the tetris ice lattice.

cond-mat.mes-hall↗

arXiv2023

First-order phase transition vs. spin-state quantum-critical scenarios in strain-tuned epitaxial cobaltite thin films

Pr-containing perovskite cobaltites exhibit unusual valence transitions, coupled to coincident structural, spin-state, and metal-insulator transitions. Heteroepitaxial strain was recently used to control these phenomena in the model (Pr$_{1-y}$Y$_y$)$_{1-x}$Ca$_x$CoO$_{3-\delta}$ system, stabilizing a nonmagnetic insulating phase under compression (with a room-temperature valence/spin-state/metal-insulator transition) and a ferromagnetic metallic phase under tension, thus exposing a potential spin-state quantum critical point. The latter has been proposed in cobaltites and can be probed in this system as a function of a disorder-free variable (strain). We study this here via thickness-dependent strain relaxation in compressive SrLaAlO$_4$(001)/(Pr$_{0.85}$Y$_{0.15}$)$_{0.70}$Ca$_{0.30}$CoO$_{3-\delta}$ epitaxial thin films to quasi-continuously probe structural, electronic, and magnetic behaviors across the nonmagnetic-insulator/ferromagnetic-metal boundary. High-resolution X-ray diffraction, electronic transport, magnetometry, polarized neutron reflectometry, and temperature-dependent magnetic force microscopy provide a detailed picture, including abundant evidence of temperature- and strain-dependent phase coexistence. This indicates a first-order phase transition as opposed to spin-state quantum-critical behavior, which we discuss theoretically via a phenomenological Landau model for coupled spin-state and magnetic phase transitions.

cond-mat.str-el↗

arXiv2022

Collective ferromagnetism of artificial square spin ice

We have studied the temperature and magnetic field dependence of the total magnetic moment of large-area permalloy artificial square spin ice arrays. The temperature dependence and hysteresis behavior are consistent with the coherent magnetization reversal expected in the Stoner-Wohlfarth model, with clear deviations due to inter-island interactions at small lattice spacing. Through micromagnetic simulations, we explore this behavior and demonstrate that the deviations result from increasingly complex magnetization reversal at small lattice spacing, induced by inter-island interactions, and depending critically on details of the island shapes. These results establish new means to tune the physical properties of artificial spin ice structures and other interacting nanomagnet systems, such as patterned magnetic media.

cond-mat.mes-hall↗

arXiv2022

Magnetic-Field-Dependent Thermodynamic Properties of Square and Quadrupolar Artificial Spin Ice

Applied magnetic fields are an important tuning parameter for artificial spin ice (ASI) systems, as they can drive phase transitions between different magnetic ground states, or tune through regimes with high populations of emergent magnetic excitations (e.g., monopole-like quasiparticles). Here, using simulations supported by experiments, we investigate the thermodynamic properties and magnetic phases of square and quadrupolar ASI as a function of applied in-plane magnetic fields. Monte Carlo simulations are used to generate field-dependent maps of the magnetization, the magnetic specific heat, the thermodynamic magnetization fluctuations, and the magnetic order parameters, all under equilibrium conditions. These maps reveal the diversity of magnetic orderings and the phase transitions that occur in different regions of the phase diagrams of these ASIs, and are experimentally supported by magneto-optical measurements of the equilibrium "magnetization noise" in thermally-active ASIs.

cond-mat.mes-hall↗

arXiv2021

Experimental Realization of the 1D Random Field Ising Model

We have measured magnetic-field-induced avalanches in a square artificial spin ice array of interacting nanomagnets. Starting from the ground state ordered configuration, we imaged the individual nanomagnet moments after each successive application of an incrementally increasing field. The statistics of the evolution of the moment configuration show good agreement with the canonical one-dimensional random field Ising model. We extract information about the microscopic structure of the arrays from our macroscopic measurements of their collective behavior, demonstrating a process that could be applied to other systems exhibiting avalanches.

cond-mat.mes-hall↗

arXiv2021

The essential role of magnetic frustration in the phase diagrams of doped cobaltites

Doped perovskite cobaltites (e.g., La$_{1-x}$Sr$_x$CoO$_3$) have been extensively studied for their spin-state physics, electronic inhomogeneity, and insulator-metal transitions. Ferromagnetically-interacting spin-state polarons emerge at low $x$ in the phase diagram of these compounds, eventually yielding long-range ferromagnetism. The onset of long-range ferromagnetism ($x \approx 0.18$) is substantially delayed relative to polaron percolation ($x \approx 0.05$), however, generating a troubling inconsistency. Here, Monte-Carlo simulations of a disordered classical spin model are used to establish that previously ignored magnetic frustration is responsible for this effect, enabling faithful reproduction of the magnetic phase diagram.

cond-mat.str-el↗

arXiv2021

Ferroelectric quantum criticality and enhanced superconductivity in plastically deformed strontium titanate

The properties of quantum materials are commonly tuned using experimental variables such as pressure, magnetic field and doping. Here we explore a different approach: irreversible, plastic deformation of single crystals. We show for the superconductor SrTiO$_3$ that compressive plastic deformation induces low-dimensional superconductivity significantly above the superconducting transition temperature ($T_c$) of undeformed samples, with evidence of superconducting correlations at temperatures two orders of magnitude above the bulk $T_c$. The superconductivity enhancement is correlated with the appearance of self-organized dislocation structures, as revealed by diffuse neutron and X-ray scattering. We also observe signatures of deformation-induced quantum-critical ferroelectric fluctuations and inhomogeneous ferroelectric order via Raman scattering. These results suggest that the strain surrounding the self-organized dislocation structures induces local ferroelectricity and quantum-critical dynamics that strongly influence $T_c$, consistent with a theory of superconductivity enhanced by soft polar fluctuations. More broadly, our results demonstrate the promise of plastic deformation and dislocation engineering as tools to manipulate electronic properties of quantum materials.

cond-mat.supr-con↗

arXiv2021

Nature of the ferromagnetic-antiferromagnetic transition in Y$_{1-x}$La$_{x}$TiO$_{3}$

We explore the magnetically-ordered ground state of the isovalently-substituted Mott-insulator Y$_{1-x}$La$_{x}$TiO$_{3}$ for $x$ $\leq$ 0.3 via single crystal growth, magnetometry, neutron diffraction, x-ray magnetic circular dichroism (XMCD), muon spin rotation ($μ$SR) and small-angle neutron scattering (SANS). We find that the decrease in the magnetic transition temperature on approaching the ferromagnetic (FM) - antiferromagnetic (AFM) phase boundary at the La concentration $x_c$ $\approx$ 0.3 is accompanied by a strong suppression of both bulk and local ordered magnetic moments, along with a volume-wise separation into magnetically-ordered and paramagnetic regions. The thermal phase transition does not show conventional second-order behavior, since neither a clear signature of dynamic critical behavior nor a power-law divergence of the magnetic correlation length is found for the studied substitution range; this finding becomes increasingly obvious with substitution. Finally, from SANS and magnetometry measurements, we discern a crossover from easy-axis to easy-plane magneto-crystalline anisotropy with increasing La substitution. These results indicate complex changes in magnetic structure upon approaching the phase boundary.

cond-mat.str-el↗

arXiv2020

Field-Induced Magnetic Monopole Plasma in Artificial Spin Ice

Artificial spin ices (ASIs) are interacting arrays of lithographically-defined nanomagnets in which novel frustrated magnetic phases can be intentionally designed. A key emergent description of fundamental excitations in ASIs is that of magnetic monopoles -- mobile quasiparticles that carry an effective magnetic charge. Here we demonstrate that the archetypal square ASI lattice can host, in specific regions of its magnetic phase diagram, high-density plasma-like regimes of mobile magnetic monopoles. By passively "listening" to spontaneous monopole noise in thermal equilibrium, we reveal their intrinsic dynamics and show that monopole kinetics are minimally correlated (that is, most diffusive) in the plasma phase. These results open the door to on-demand monopole regimes having field-tunable densities and dynamic properties, thereby providing a new paradigm for probing the physics of effective magnetic charges in synthetic matter.

cond-mat.mes-hall↗

arXiv2019

Low Temperature Specific Heat of Doped SrTiO$_3$: Doping Dependence of the Effective Mass and Kadowaki-Woods Scaling Violation

We report wide-doping-range ($8 \times 10^{17}$ to $4 \times 10^{20}$ cm$^{-3}$ Hall electron density) low temperature specific heat measurements on single crystal SrTiO$_3$:Nb, correlated with electronic transport data and tight-binding modeling. Lattice dynamic contributions to specific heat are shown to be well understood, albeit with unusual sensitivity to doping, likely related to the behavior of soft modes. Electronic contributions to specific heat provide effective masses that increase substantially, from $1.8$ to $4.8 m_e$, across the two SrTiO$_3$ Lifshitz transitions. It is shown that this behavior can be quantitatively reconciled with quantum oscillation data and calculated band structure, establishing a remarkably doping-independent mass enhancement factor of $2.0$. Most importantly, with the doping-dependent $T^2$ resistivity prefactor and Sommerfeld coefficient known, Kadowaki-Woods scaling has been tested over the entire doping range probed. Despite classic Fermi liquid behavior in electronic specific heat, standard Kadowaki-Woods scaling is dramatically violated, highlighting the need for new theoretical descriptions of $T^2$ resistivity in SrTiO$_3$.

cond-mat.str-el↗

arXiv2016

Percolation via combined electrostatic and chemical doping in complex oxide films

Stimulated by experimental advances in electrolyte gating methods, we investigate theoretically percolation in thin films of inhomogenous complex oxides, such as La$_{1-x}$Sr$_{x}$CoO$_{3}$ (LSCO), induced by a combination of bulk chemical and surface electrostatic doping. Using numerical and analytical methods, we identify two mechanisms that describe how bulk dopants reduce the amount of electrostatic surface charge required to reach percolation: (i) bulk-assisted surface percolation, and (ii) surface-assisted bulk percolation. We show that the critical surface charge strongly depends on the film thickness when the film is close to the chemical percolation threshold. In particular, thin films can be driven across the percolation transition by modest surface charge densities \emph{via} surface-assisted bulk percolation. If percolation is associated with the onset of ferromagnetism, as in LSCO, we further demonstrate that the presence of critical magnetic clusters extending from the film surface into the bulk results in considerable volume enhancement of the saturation magnetization, with pronounced experimental consequences. These results should significantly guide experimental work seeking to verify gate-induced percolation transitions in such materials.

cond-mat.mes-hall↗

arXiv2016

First-principles study of crystal and electronic structure of rare-earth cobaltites

Using density functional theory plus self-consistent Hubbard $U$ (DFT$+U_{sc}$) calculations, we have investigated the structural and electronic properties of the rare-earth cobaltites \textit{R}CoO$_3$ (\textit{R} = Pr -- Lu). Our calculations show the evolution of crystal and electronic structure of the insulating low-spin (LS) \textit{R}CoO$_3$ with increasing rare-earth atomic number (decreasing ionic radius), including the invariance of the Co-O bond distance ($d_{Co-O}$), the decrease of the Co-O-Co bond angle ($Θ$), and the increase of the crystal field splitting ($Δ_{CF}$) and band gap energy ($E_g$). Agreement with experiment for the latter improves considerably with the use of DFT$+U_{sc}$ and all trends are in good agreement with experimental data. These trends enable a direct test of prior rationalizations of the trend in spin-gap associated with the spin crossover in this series, which is found to expose significant issues with simple band based arguments. We also examine the effect of placing the rare-earth \textit{f}-electrons in the core region of the pseudopotential. The effect on lattice parameters and band structure is found to be small, but distinct for the special case of \textit{Pr}CoO$_3$ where some \textit{f}-states populate the middle of the gap, consistent with recent reports of unique behavior in Pr-containing cobaltites. Overall, this study establishes a foundation for future predictive studies of thermally induced spin excitations in rare-earth cobaltites and similar systems.

cond-mat.str-el↗

arXiv2016

Phase Separation and Superparamagnetism in the Martensitic Phase of $Ni_{50-x}Co_{x}Mn_{40}Sn_{10}$

$Ni_{50-x}Co_{x}Mn_{40}Sn_{10}$ shape memory alloys in the approximate range $5 \le x \le 10$ display desirable properties for applications as well as intriguing magnetism. These off-stoichiometric Heusler alloys undergo a martensitic phase transformation at a temperature $T_{M}$ of 300 - 400 K, from ferromagnetic (F) to nonferromagnetic, with unusually low thermal hysteresis and a large change in magnetization. The low temperature magnetic structures in the martensitic phase of such alloys, which are distinctly inhomogeneous, are of great interest but are not well understood. Our present use of spin echo NMR, in the large hyperfine fields at $^{55}Mn$ sites, provides compelling evidence that nanoscale magnetic phase separation into F and antiferromagnetic (AF) regions occurs below $T_{M}$ in alloys with x in the range 0 to 7. At finite Co substitution the F regions are found to be of two distinct types, corresponding to high and low local concentrations of Co on Ni sites. Estimates of the size distributions of both the F and AF nanoregions have been made. At x = 7 the AF component is not long-range ordered, even below 4 K, and is quite different to the AF component found at x = 0; by x = 14 the F phase is completely dominant. Of particular interest, we find, for x = 7, that field cooling leads to dramatic changes in the AF regions. These findings provide insight into the origins of magnetic phase separation and superparamagnetism in these complex alloys, particularly their intrinsic exchange bias, which is of considerable current interest.

cond-mat.mtrl-sci↗

arXiv2014

Revealing Optically Induced Magnetization in SrTiO$_3$ using Optically Coupled SQUID Magnetometry and Magnetic Circular Dichroism

In this work, we study the time- and temperature-dependence of optically induced magnetization in bulk crystals of slightly oxygen-deficient SrTiO$_{3-δ}$ using an optically coupled SQUID magnetometer. We find that a weak ($\sim$5$\times$10$^{-7}$~emu) but extremely long-lived (hours) magnetic moment can be induced in SrTiO$_{3-δ}$ at zero magnetic field by circular-polarized sub-bandgap light. We utilize this effect to demonstrate that SrTiO$_{3-δ}$ crystals can be used as an optically addressable magnetic memory by writing and subsequently reading magnetic patterns with light. The induced magnetization is consistent with that of a polarized ensemble of independent oxygen-vacancy-related complexes, rather than from collective or long-range magnetic order.

cond-mat.mtrl-sci↗

arXiv2014

Persistent Optically Induced Magnetism in Oxygen-Deficient Strontium Titanate

Strontium titanate (SrTiO$_3$) is a foundational material in the emerging field of complex oxide electronics. While its electronic and optical properties have been studied for decades, SrTiO$_3$ has recently become a renewed materials research focus catalyzed in part by the discovery of magnetism and superconductivity at interfaces between SrTiO$_3$ and other oxides. The formation and distribution of oxygen vacancies may play an essential but as-yet-incompletely understood role in these effects. Moreover, recent signatures of magnetization in gated SrTiO$_3$ have further galvanized interest in the emergent properties of this nominally nonmagnetic material. Here we observe an optically induced and persistent magnetization in oxygen-deficient SrTiO$_{3-δ}$ using magnetic circular dichroism (MCD) spectroscopy and SQUID magnetometry. This zero-field magnetization appears below ~18K, persists for hours below 10K, and is tunable via the polarization and wavelength of sub-bandgap (400-500nm) light. These effects occur only in oxygen-deficient samples, revealing the detailed interplay between magnetism, lattice defects, and light in an archetypal oxide material.

cond-mat.mes-hall↗

arXiv2012

Perpendicular Magnetization and Generic Realization of the Ising Model in Artificial Spin Ice

We have studied frustrated kagome arrays and unfrustrated honeycomb arrays of magnetostatically-interacting single-domain ferromagnetic islands with magnetization normal to the plane. The measured pairwise spin correlations of both lattices can be reproduced by models based solely on nearest-neighbor correlations. The kagome array has qualitatively different magnetostatics but identical lattice topology to previously-studied 'artificial spin ice' systems composed of in-plane moments. The two systems show striking similarities in the development of moment pair correlations, demonstrating a universality in artificial spin ice behavior independent of specific realization in a particular material system.

cond-mat.mes-hall↗

arXiv2011

RbFe2+Fe3+F6: Synthesis, Structure, and Characterization of a New Charge-Ordered Magnetically Frustrated Pyrochlore-Related Mixed-Metal Fluoride

A new charge-ordered magnetically frustrated mixed-metal fluoride with a pyrochlore-related structure has been synthesized and characterized. The material, RbFe2F6 (RbFe2+Fe3+F6) was synthesized through mild hydrothermal conditions. The material exhibits a three-dimensional pyrochlore-related structure consisting of corner-shared Fe2+F6 and Fe3+F6 octahedra. In addition to single crystal diffraction data, neutron powder diffraction and magnetometry measurements were carried out. Magnetic data clearly reveal strong antiferromagnetic interactions (a Curie-Weiss temperature of -270 K) but sufficient frustration to prevent ordering until 16 K. No structural phase transformation is detected from the variable temperature neutron diffraction data. Infrared, UV -vis, thermogravimetric, and differential thermal analysis measurements were also performed. First-principles density functional theory (DFT) electronic structure calculations were also done. Crystal data: RbFe2F6, orthorhombic, space group Pnma (No. 62), a = 7.0177(6) Å, b = 7.4499(6) Å, c = 10.1765(8) Å, V = 532.04(8) Å3, Z = 4.

cond-mat.mtrl-sci↗

arXiv2009

Bulk Spin Polarization of Co$_{(1-x)}$Fe$_x$S$_2$

We report on a new method to determine the degree of bulk spin polarization in single crystal Co$_{(1-x)}$Fe$_x$S$_2$ by modeling magnetic Compton scattering with {\it ab initio} calculations. Spin-dependent Compton profiles were measured for CoS$_2$ and Co$_{0.9}$Fe$_{0.1}$S$_2$. The {\it ab initio} calculations were then refined by rigidly shifting the bands to provide the best fit between the calculated and experimental directional profiles for each sample. The bulk spin polarizations, $P$, corresponding to the spin-polarized density of states at the Fermi level, were then extracted from the {\it refined} calculations. The values were found to be $P=-72 \pm 6 %$ and $P=18 \pm 7%$ for CoS$_2$ and Co$_{0.9}$Fe$_{0.1}$S$_2$ respectively. Furthermore, determinations of $P$ weighted by the Fermi velocity ($v_F$ or $v_F^2$) were obtained, permitting a rigorous comparison with other experimental data and highlighting the experimental dependence of $P$ on $v_F$.

cond-mat.str-el↗