arXiv subjects

John T. Heron

Publications and source records attributed to John T. Heron.

At least 19 recordsLinked to original sources

arXiv2026

Anomalous Crystallinity and Magnetism in Chemically Disordered Coherent Heterostructures

High-entropy oxide (HEO) thin films uniquely superimpose exceptional chemical disorder with exceptional crystalline quality and coherence - an intersection we term anomalous crystallinity that arises from coupled structural, chemical, and valence degrees of freedom unique to the entropy-stabilized condition. Here, we demonstrate unexpected and predictive control of this state using formulation, epitaxial constraints, and kinetic arrest of metastable macrostates. Specifically, aliovalent cation substitutions, tightly controlled substrate temperatures, and conditions favoring significant adatom kinetic energy, can program the out-of-plane lattice parameter of coherent rock salt HEOs while preserving in-plane epitaxial pinning to MgO. Lattice strains exceeding 5% can be stabilized in multilayer heterostructures using this approach, where 3+ cations compensated by cation vacancies predominate the defect chemistry landscape. We highlight the exemplar (Sc,Mg,Co,Ni,Cu,Zn)O/(Cr,Mg,Co,Ni,Cu,Zn)O (JSc/JCr) system where Sc and Cr substitution into the rock salt structure produces pseudomorphic heterostructures between individual antiferromagnets exhibiting exceptional strain and abrupt interfaces across which the Co valence switches from mostly 2+ to an even 2+/3+ mixture. These unprecedented valence interfaces are accompanied by a 2x exchange bias boost compared to single-layer constituents, that could be attributed to enhanced uncompensated spins in the layers themselves or around the buried JSc/JCr interface. These results establish pseudomorphic valence interfaces with anomalous crystallinity as a source of new magnetic macrostates that host emergent magnetic and spintronic functionality.

cond-mat.mtrl-sci↗

arXiv2026

Ferroelectric dynamic-field-driven nucleation and growth model for predictive materials-to-circuit co-design

Real ferroelectric devices operate under mixed and distorted time-varying voltages, yet the standard nucleation-growth frameworks used to interpret ferroelectric switching - most notably the Kolmogorov-Avrami-Ishibashi (KAI) and nucleation-limited switching models (NLS) - are derived under the critically limiting assumption of a constant electric field. Thus, the prevailing interpretation of ferroelectric switching dynamics fails under real operating conditions. Here we introduce a compact dynamic-field-driven nucleation and growth (DFNG) model that enables quantitative fits to switching transients across multiple ferroelectric materials to extract time-varying domain wall velocity and growth dimensionality, even under arbitrary voltage waveform. This capability then motivates its use in device modeling under complex signals spanning disparate time and frequency scales. Coupling the compact model to application-related waveforms and circuit-level simulation platform facilitates a predictive materials-circuit co-design framework by linking nucleation and growth parameters to memory window, disturb error, speed, and energy dissipation for next-generation ferroelectric technologies.

cond-mat.mtrl-sci↗

arXiv2026

Historical Foundation and Practical Guideline for Ferroelectric Switching Kinetic Studies

Electrical measurements of ferroelectric switching kinetics are widely used to probe the dynamics of polarization reversal, yet the influence of the measurement circuit is often underappreciated. In this paper, we show that the interplay between ferroelectric capacitors and circuit elements produces distorted, time-dependent voltage waveforms across the device, particularly in the sub-ns regime. We examine how these circuit contributions affect polarization transients extracted from PUND measurements. The resulting distortions scale with supply voltage, capacitor dimensions, and lumped circuit elements, but are not accounted for in conventional experimental analyses or analytical model fitting. We then critically assess existing nucleation and growth models and show that neglecting the time-varying voltage profile can lead to unphysical interpretations of switching kinetics, most notably in the extracted growth dimensionality represented by the Avrami exponent. Finally, we outline guidelines for future studies, emphasizing the need for direct voltage monitoring and circuit-aware de-embedding, as well as modeling frameworks that incorporate voltage-dependent nucleation and growth rates based on intrinsic material parameters.

cond-mat.mtrl-sci↗

arXiv2026

Optimizing Flux Method Growth of Rutile GeO2 Crystals

Rutile germanium oxide (r-GeO2) has shown potential for ultrawide bandgap semiconductor applications such as power conversion and UV optoelectronics. Homoepitaxial substrates will be key for achieving phase pure and doped r-GeO2 thin films as synthesis is inhibited by strain associated with substrate lattice mismatch. Initial reports of single crystal r-GeO2 synthesis from a MoO3-Li2CO3 flux have shown mm scale crystals with dominantly (110) faceting. However, fundamental understanding of the synthesis parameters and the ability to tune size and facet are needed. Here, we report on both seeded and unseeded growth of single crystal r-GeO2 across a range of MoO3-Li2CO3 flux compositions. Small variations in Mo concentration can be used to control crystal habit, faceting, and growth rate through variation in precursor complexion, solution viscosity, and GeO2 solubility. While seed size and seeded growth rates are optimized in 40% Mo solutions, aspect ratios and seeded growth volumes are maximized in 41.5% Mo solutions without sacrificing faceting. Increased Mo concentration leads to polycrystallinity and isotropic growth. These results enable faster and tailored growth of r-GeO2 crystals using the flux growth method.

cond-mat.mtrl-sci↗

arXiv2026

The Evolution of Magnetism in a Thin Film Pyrochlore Ferromagnetic Insulator

The pyrochlore vanadates are compelling candidates for next-generation dissipationless devices. Lu2V2O7 and Y2V2O7 are ferromagnetic insulators (Tc ~ 70 K) that are believed to exhibit the magnon Hall effect and are expected to host topological magnons. Their completely dissipationless magnon edge states could be harnessed to realize low-power information transport in spintronic or magnonic devices. As a crucial step in the realization of devices, we synthesize the first thin films of pyrochlore Y2V2O7 on isostructural Y2Ti2O7 substrates and explore the evolution of their magnetic properties down to the ultrathin limit. All films are insulating ferromagnets with transition temperatures of up to the bulk value (Tc ~ 68 K) that decrease with thickness according to finite-size effects. Our films also exhibit a change in anisotropy from in-plane to out-of-plane easy axis coincident with the development of partial strain relaxation and nonzero magnetic hysteresis in an applied field. This evolution demonstrates the impact of strain on magnetic anisotropy and paves the way to tunable magnon topology.

cond-mat.mtrl-sci↗

arXiv2026

Gilbert Damping Parameters of Epitaxially-Stabilized Iron Gallium Thin Films from Ferromagnetic Resonance

Iron gallium (FeGa) alloys are excellent rare-earth-free magnetostrictors. Through epitaxial stabilization, the disordered A2 alloy can be extended from 19% to 30% gallium resulting in a magnetostrictive coefficient almost twice than that which is seen in rare earth magnetostrictors like SmFe2. In a composite magnetoelectric structure, this makes epitaxially-stabilized iron gallium a key material for energy-efficient beyond CMOS technologies. The energy dissipation and speed of magnetoelectric switching, however, is affected by the magnetic resonance frequency and damping. Here we report the evolution of the ferromagnetic resonance and key materials parameters (magnetic anisotropy, magnetic damping, and magnetostriction coefficient) for 70 nm thick epitaxially-stabilized single crystal A2 FeGa films beyond 19% Ga. Using flip chip ferromagnetic resonance (1-14 GHz), we find that the Gilbert damping parameter spans the range of 0.09-0.16 and decreases as the Ga concentration increases. This correlates an increasing magnetoelastic coupling with a reduction in the Gilbert damping. We find that the effective damping is a mix of contributions from the intrinsic magnon-phonon scattering and other scattering/dissipation mechanisms, with the latter being dominant especially at high Ga composition. Our results provide insight into the mechanism of magnetic relaxation in metastable high magnetostriction materials and potential switching behavior of composite magnetoelectrics.

cond-mat.mtrl-sci↗

arXiv2025

Intertwined polar, chiral, and ferro-rotational orders in a rotation-only insulator

Intertwined orders refer to strongly coupled and mutually dependent orders that coexist in correlated electron systems, often underpinning key physical properties of the host materials. Among them, polar, chiral, and ferro-rotational orders have been theoretically known to form a closed set of intertwined orders. However, experimental investigation into their mutual coupling and physical consequences has remained elusive. In this work, we employ the polar-chiral insulator Ni$_3$TeO$_6$ as a platform and utilize a multimodal optical approach to directly probe and reveal the intertwining among polarity, chirality, and ferro-rotational order. We demonstrate how their coupling governs the formation of domains and dictates the nature of domain walls. Within the domains, we identify spatial inversion symmetry as the operation connecting two domain states of opposite polarity and chirality, with a common ferro-rotational state serving as the prerequisite for these interlocked configurations. At the domain walls, we observe a pronounced enhancement of in-plane polarization accompanied by a suppression of chirality. By combining with Ginzburg-Landau theory within the framework of a pre-existing ferro-rotational background, we uncover the emergence of mixed Néel- and Bloch-type domain walls. Our findings highlight the critical role of intertwined orders in defining domain and domain wall characteristics and open pathways for domain switching and domain wall control via intertwined order parameters.

cond-mat.mtrl-sci↗

arXiv2025

Material-Limited Switching in Nanoscale Ferroelectrics

The ferroelectric switching speed has been experimentally obfuscated by the interaction between the measurement circuit and the ferroelectric switching itself. This has prohibited the observation of real material responses at nanosecond timescales and lower. Here, fundamental polarization switching speeds in ferroelectric materials with the perovskite, fluorite, and wurtzite structures are reported. Upon lateral scaling of island capacitors from micron to nanoscales, a clear transition from circuit-limited switching to a material-limited switching regime is observed. In La$_{0.15}$Bi$_{0.85}$FeO$_{3}$ capacitors, switching is as fast as ~150 ps, the fastest switching time reported. For polycrystalline Hf$_{0.5}$Zr$_{0.5}$O$_{2}$ capacitors, a fundamental switching limit of ~210 ps is observed. Switching times for Al$_{0.92}$B$_{0.08}$N are near 20 ns, limited by the coercive and breakdown electric fields. The activation field, instantaneous pseudo-resistivity, and energy-delay are reported in this material-limited regime. Lastly, a criterion for reaching the material-limited regime is provided. This regime enables observation of intrinsic material properties and favorable scaling trends for high-performance computing.

cond-mat.mtrl-sci↗

arXiv2025

Chemically-Disordered Transparent Conductive Perovskites with High Crystalline Fidelity

This manuscript presents a working model linking chemical disorder and transport properties in correlated-electron perovskites with high-entropy formulations and a framework to actively design them. We demonstrate this new learning in epitaxial Sr$x$(Ti,Cr,Nb,Mo,W)O$3$ thin films that exhibit exceptional crystalline fidelity despite a diverse chemical formulation where most B-site species are highly misfit with respect to valence and radius. X-ray diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy confirm a unique combination of chemical disorder and structural perfection in thick epitaxial layers. This combination produces significant electron correlation, low electrical resistivity, and an optical transparency window that surpasses that of constituent end-members, with a flattened frequency- and temperature-dependent response. We address the computational challenges of modeling such systems and investigate short-range ordering using cluster expansion. These results showcase that unusual d-metal combinations access an expanded property design space that is predictable using end-member characteristics -- though unavailable to them -- thus offering performance advances in optical, spintronic, and quantum devices.

cond-mat.mtrl-sci↗

arXiv2025

Extreme-Band-Gap Semiconductors with Shallow Dopants and Mobile Carriers

The conventional distinction between semiconductors and insulators is often based on the magnitude of the band gap, with materials exhibiting gaps wider than 3 eV typically classified as insulators. However, the emergence of ultra-wide-band-gap (UWBG) semiconductors such as AlGaN, diamond, BN, and Ga2O3 challenges this paradigm for materials classification and raises fundamental questions about the upper bound of band gaps compatible with semiconducting behavior. Here we develop a computational-discovery strategy to identify semiconductors with band gaps exceeding that of AlN (6.2 eV), while retaining essential semiconducting properties such as shallow dopants and mobile charge carriers. We discover that materials composed of light elements in densely packed crystal structures exhibit wide band gaps and light carrier effective masses that enable shallow dopants, high mobility, and weak polaron binding. By applying the hydrogenic Bohr model and first-principles defect calculations - validated against available experimental data - to screen for materials with shallow dopants, we identify dopable compounds with gaps as wide as 9.5 eV that nonetheless host mobile charge carriers. Our findings demonstrate that semiconducting behavior persists even at extreme band gaps, far beyond conventional upper bounds traditionally associated with semiconductor materials.

cond-mat.mtrl-sci↗

arXiv2024

Local structure maturation in high entropy oxide (Mg,Co,Ni,Cu,Zn)1-x(Cr,Mn)xO thin films

High entropy oxides (HEO)s have garnered much interest due to their available high degree of tunability. Here, we study the local structure of (MgNiCuCoZn)0.167(MnCr)0.083O, a composition based on the parent HEO (MgNiCuCoZn)0.2O.We synthesized a series of thin films via pulsed laser deposition at incremental oxygen partial pressures. X-ray diffraction shows lattice parameter to decrease with increased pO2 pressures until the onset of phase separation. X-ray absorption fine structure shows that specific atomic species in the composition dictate the global structure of the material as Cr, Co, and Mn shift to energetically favorable coordination with increasing pressure. Transmission electron microscopy analysis on a lower-pressure sample exhibits a rock salt structure, but the higher-pressure sample reveals reflections reminiscent of the spinel structure. In all, these findings give a more complete picture on how (MgNiCuCoZn)0.167(MnCr)0.083O forms with varying initial conditions and advances fundamental knowledge of cation behavior in high entropy oxides.

cond-mat.mtrl-sci↗

arXiv2024

Untangling individual cation roles in rock salt high-entropy oxides

We unravel the distinct roles each cation plays in phase evolution, stability, and properties within Mg1/5Co1/5Ni1/5Cu1/5Zn1/5O high-entropy oxide (HEO) by integrating experimental findings, thermodynamic analyses, and first-principles predictions. Our approach is through sequentially removing one cation at a time from the five-component high-entropy oxide to create five four-component derivatives. Bulk synthesis experiments indicate that Mg, Ni, and Co act as rock salt phase stabilizers whereas only Mg and Ni enthalpically enhance single-phase rock salt stability in thin film growth; synthesis conditions dictate whether Co is a rock salt phase stabilizer or destabilizer. By examining the competing phases and oxidation state preferences using pseudo-binary phase diagrams and first-principles calculations, we resolve the stability differences between bulk and thin film for all compositions. We systematically explore HEO macroscopic property sensitivity to cation selection employing both predicted and measured optical spectra. This study establishes a framework for understanding high-entropy oxide synthesizability and properties on a per-cation basis that is broadly applicable to tailoring functional property design in other high-entropy materials.

cond-mat.mtrl-sci↗

arXiv2023

Endotaxial Stabilization of 2D Charge Density Waves with Long-range Order

Charge density waves are emergent quantum states that spontaneously reduce crystal symmetry, drive metal-insulator transitions, and precede superconductivity. In low-dimensions, distinct quantum states arise, however, thermal fluctuations and external disorder destroy long-range order. Here we stabilize ordered two-dimensional (2D) charge density waves through endotaxial synthesis of confined monolayers of 1T-TaS$_2$. Specifically, an ordered incommensurate charge density wave (oIC-CDW) is realized in 2D with dramatically enhanced amplitude and resistivity. By enhancing CDW order, the hexatic nature of charge density waves becomes observable. Upon heating via in-situ TEM, the CDW continuously melts in a reversible hexatic process wherein topological defects form in the charge density wave. From these results, new regimes of the CDW phase diagram for 1T-TaS$_2$ are derived and consistent with the predicted emergence of vestigial quantum order.

cond-mat.mtrl-sci↗

arXiv2022

Antiferromagnetic metal phase in an electron-doped rare-earth nickelate

Long viewed as passive elements, antiferromagnetic materials have emerged as promising candidates for spintronic devices due to their insensitivity to external fields and potential for high-speed switching. Recent work exploiting spin and orbital effects has identified ways to electrically control and probe the spins in metallic antiferromagnets, especially in noncollinear or noncentrosymmetric spin structures. The rare earth nickelate NdNiO3 is known to be a noncollinear antiferromagnet where the onset of antiferromagnetic ordering is concomitant with a transition to an insulating state. Here, we find that for low electron doping, the magnetic order on the nickel site is preserved while electronically a new metallic phase is induced. We show that this metallic phase has a Fermi surface that is mostly gapped by an electronic reconstruction driven by the bond disproportionation. Furthermore, we demonstrate the ability to write to and read from the spin structure via a large zero-field planar Hall effect. Our results expand the already rich phase diagram of the rare-earth nickelates and may enable spintronics applications in this family of correlated oxides.

cond-mat.str-el↗

arXiv2022

Two-dimensional charge order stabilized in clean polytype heterostructures

Compelling evidence suggests distinct correlated electron behavior may exist only in clean 2D materials such as 1T-TaS2. Unfortunately, experiment and theory suggest that extrinsic disorder in free standing 2D layers disrupts correlation-driven quantum behavior. Here we demonstrate a route to realizing fragile 2D quantum states through endotaxial polytype engineering of van der Waals materials. The true isolation of 2D charge density waves (CDWs) between metallic layers stabilizes commensurate long-range order and lifts the coupling between neighboring CDW layers to restore mirror symmetries via interlayer CDW twinning. The twinned-commensurate charge density wave (tC-CDW) reported herein has a single metal--insulator phase transition at ~350 K as measured structurally and electronically. Fast in-situ transmission electron microscopy and scanned nanobeam diffraction map the formation of tC-CDWs. This work introduces endotaxial polytype engineering of van der Waals materials to access latent 2D ground states distinct from conventional 2D fabrication.

cond-mat.mtrl-sci↗

arXiv2021

A Narrowband Spintronic Terahertz Emitter based on Magnetoelastic Heterostructures

Narrowband terahertz (THz) radiation is crucial for high-resolution spectral identification, but a narrowband THz source driven by femtosecond (fs) laser has remained scarce. Here, it is computationally predicted that a metal/dielectric/magnetoelastic heterostructure enables converting a fs laser pulse into a multi-cycle THz pulse with a narrow linewidth down to ~1.5 GHz, which is in contrast with the single-cycle, broadband THz pulse from the existing fs-laser-excited emitters. It is shown that such narrowband THz pulse originates from the excitation and long-distance transport of THz spin waves in the magnetoelastic film, which can be enabled by a short strain pulse obtained from fs laser irradiation of the metal film when the thicknesses of the metal and magnetoelastic films both fall into a specific range. These results therefore reveal an approach to achieving optical generation of narrowband THz pulse based on heterostructure design, which also has implications in the design of THz magnonic devices.

cond-mat.mes-hall↗

arXiv2021

Superconductivity in a quintuple-layer square-planar nickelate

Since the discovery of high-temperature superconductivity in the copper oxide materials, there have been sustained efforts to both understand the origins of this phase and discover new cuprate-like superconducting materials. One prime materials platform has been the rare-earth nickelates and indeed superconductivity was recently discovered in the doped compound Nd$_{0.8}$Sr$_{0.2}$NiO$_2$. Undoped NdNiO$_2$ belongs to a series of layered square-planar nickelates with chemical formula Nd$_{n+1}$Ni$_n$O$_{2n+2}$ and is known as the 'infinite-layer' ($n = \infty$) nickelate. Here, we report the synthesis of the quintuple-layer ($n = 5$) member of this series, Nd$_6$Ni$_5$O$_{12}$, in which optimal cuprate-like electron filling ($d^{8.8}$) is achieved without chemical doping. We observe a superconducting transition beginning at $\sim$13 K. Electronic structure calculations, in tandem with magnetoresistive and spectroscopic measurements, suggest that Nd$_6$Ni$_5$O$_{12}$ interpolates between cuprate-like and infinite-layer nickelate-like behavior. In engineering a distinct superconducting nickelate, we identify the square-planar nickelates as a new family of superconductors which can be tuned via both doping and dimensionality.

cond-mat.supr-con↗

arXiv2019

Imaging uncompensated moments and exchange-biased emergent ferromagnetism in FeRh thin films

Uncompensated moments in antiferromagnets are responsible for exchange bias in antiferromagnet/ferromagnet heterostructures; however, they are difficult to directly detect because any signal they contribute is typically overwhelmed by the ferromagnetic layer. We use magneto-thermal microscopy to image uncompensated moments in thin films of FeRh, a room-temperature antiferromagnet that exhibits a 1st-order phase transition to a ferromagnetic state near 100~$^\circ$C. FeRh provides the unique opportunity to study both uncompensated moments in the antiferromagnetic phase and the interaction of uncompensated moments with emergent ferromagnetism within a relatively broad (10-15~$^\circ$C) temperature range near $T_C$. In the AF phase below $T_C$, we image both pinned UMs, which cause local vertical exchange bias, and unpinned UMs, which exhibit an enhanced coercive field that reflects exchange-coupling to the AF bulk. Near $T_C$, where AF and FM order coexist, we find that the emergent FM order is exchange-coupled to the bulk Néel order. This exchange coupling leads to the nucleation of unusual configurations in which different FM domains are pinned parallel, antiparallel, and perpendicular to the applied magnetic field before suddenly collapsing into a state uniformly parallel to the field.

cond-mat.mtrl-sci↗