arXiv subjects

Robert Hovden

Publications and source records attributed to Robert Hovden.

At least 19 recordsLinked to original sources

arXiv2026

Origin of the reaction temperature in solid-state materials synthesis

Temperature plays a crucial role in solid-state materials synthesis, but there is currently no mechanistic theory to explain or predict which temperature is best to conduct a solid-state reaction. Reactions between powder precursors are conventionally assumed to be slow diffusion-limited processes; however, recent in situ experiments show that solid-state reactions can complete in minutes above a critical onset temperature. Here, we present evidence that a transient liquid phase forms above the metastable eutectic temperature, and that this non-equilibrium liquid serves as a fast diffusion medium to intermix precursors and initiate a solid-state reaction. This thermodynamic principle is agnostic to the structure or chemistry of the reactants, and can be applied towards the synthesis and manufacturing of a wide range of complex materials.

cond-mat.mtrl-sci↗

arXiv2026

Helium-Cooled Cryogenic STEM Imaging and Ptychography for Atomic-Scale Study of Low-Temperature Phases

Much of the exotic functionality of prime interest in quantum materials emerges from structural and electronic ground states that can only be accessed at cryogenic temperatures. Understanding device operation therefore requires structural characterization under the same low-temperature conditions at which these functional phases exist, as room-temperature measurements often probe a different structural state. Achieving atomic-resolution in scanning transmission electron microscopy imaging and particularly 4D-STEM electron ptychography at liquid helium temperature has remained extremely challenging because even small amounts of drift, vibration, and thermal instability associated with the cryogen can disrupt the stringent stability requirements of atomic-resolution STEM. In this work we demonstrate atomic-resolution STEM and multislice electron ptychography at temperatures as low as 20 K using a commercial helium cooled holder. We find that rapid scans and a multi-stage registration workflow are critical to reducing artifacts associated with cryogenic instability for atomic-resolution imaging, while for ptychography scan position correction including compensation for coupling between probe aberrations and position refinement is necessary for successful reconstructions. Together these results establish a pathway for reliable atomic-resolution STEM and ptychography at low temperature, enabling direct visualization of structural ground states relevant to quantum technology.

cond-mat.mtrl-sci↗

arXiv2025

Magneto-Moiré Excitons in Twisted Bilayer CrSBr

Moiré superlattices in van der Waals materials have revolutionized the study of electronic and excitonic systems by creating periodic electrostatic potentials. Extending this concept to magnetic materials promises new pathways in merging spintronics with photonics. While moiré magnetism has been revealed with near-field probes and nonlinear optical techniques, the coupling of these magnetic textures to optical excitations - magneto-moiré excitons - remains unexplored. Here, we report the observation of magneto-moiré excitons in twisted bilayer CrSBr, correlated with moiré spin textures that emerge below a critical twist angle of ~2°. The nanoscale moiré spin texture imprints distinct signatures onto the optical spectrum, shifting the exciton energy via a periodic magnetic exchange field. First-principles calculations corroborate that these signatures arise from one-dimensional spin textures governed by the balance of exchange interactions and domain wall energy. Our results demonstrate that moiré magnetism can be used to engineer nanoscale excitonic energy landscapes, providing a new platform for magneto-optical sensing, quantum transduction, and control of non-collinear magnetism and topology through light.

cond-mat.mes-hall↗

arXiv2025

Delayed 1T to 2H Phase Transition Upon Electrochemical Delithiation of LiMoS2

Molybdenum disulfide (MoS2) is a widely studied layered material for electronic, optical, and catalytic applications. It can host lithium ions between the van der Waals layers, which triggers a phase transition between the semiconducting 2H phase and metallic 1T phase. While lithium insertion triggers a phase transition to the 1T phase, the phase behavior upon electrochemical lithium removal is not resolved. In this work, we conduct single-flake electrochemical (de)lithiation of MoS2 using microelectrode arrays. Through both electrochemical voltage analysis and correlative Raman spectroscopy, we show that an electrochemically cycled and delithiated MoS2 flake initially remains in the 1T phase. However, over the course of several days, it transitions back into the thermodynamically stable 2H phase. This result resolves the phase transformation pathway upon delithiation and showcases the ability to electrochemically synthesize the metastable 1T-MoS2 phase.

cond-mat.mtrl-sci↗

arXiv2025

Nanoscale Polar Landscapes in Quantum Paraelectric SrTiO3

SrTiO3 is a textbook quantum paraelectric, with ferroelectricity purportedly suppressed by quantum fluctuations of ionic positions down to the lowest temperatures. The precise real space structure of SrTiO3 at low temperature, however, has remained undefined despite decades of study. Here we directly image the low-temperature polar structure of quantum parelectric SrTiO3, using cryogenic scanning transmission electron microscopy down to 20 K. High resolution imaging reveals a spatially fluctuating landscape of nanoscale domains of finite polarization. The short-range polar domains first grow and self-organize into a periodic structure over tens of nanometers. However, the process reverses when entering the quantum paraelectric regime below 40 K and the periodically ordered polar nanodomains fragment into small clusters.

cond-mat.mtrl-sci↗

arXiv2025

Correlative 3D Mapping of Structure, Composition, and Valence State Dynamics in Battery Cathodes via Simultaneous ADF-EDS-EELS Tomography

Understanding degradation in battery cathodes and other functional materials requires simultaneous knowledge of structural, chemical, and electronic changes in three dimensions (3D). Here, we present a simultaneous ADF-EDS-EELS tomography method that enables 3D mapping of atomic structure, composition, valence states, and transition metal inhomogeneity within a single, low-dose STEM tilt series acquisition. Applied to LiNi1/3Co1/3Mn1/3O2 (NCM111) particles at different electrochemical cycling stages, this method reveals nanoscale degradation processes with full spatial correlation. We observe that while chemical composition evolves uniformly throughout the entire primary particle, valence state changes and transition metal segregation are strongly depth-dependent and concentrated near the surface. This coexistence of bulk and surface-driven degradation dynamics reveals distinct mechanisms acting at different spatial scales. The evolution of inhomogeneity and valence states deviates from simple phase transition models, highlighting the roles of ion migration and dissolution-driven segregation. Our findings establish valence state gradients and nanoscale inhomogeneity as active contributors to cathode failure. More broadly, this correlative 3D platform opens new opportunities for studying redox-driven transformations in fields such as neuromorphic computing and heterogeneous catalysis, where composition-structure-function coupling is inherently three-dimensional.

cond-mat.mtrl-sci↗

arXiv2025

Melting point depression of charge density wave in 1T-TiSe$_2$ due to size effects

Classical nucleation theory predicts size-dependent nucleation and melting due to surface and confinement effects at the nanoscale. In correlated electronic states, observation of size-dependent nucleation and melting is rarely reported, likely due to the extremely small length scales necessary to observe such effects for electronic states. Here, using 1T-TiSe$_2$ nanoflakes as a prototypical two-dimensional (2D) charge density wave (CDW) system, we perform in-situ cryogenic electron microscopy with temperature down to 20 K and observe size-dependent nucleation and melting of CDWs. Specifically, we observe a melting point depression of CDW for 1T-TiSe$_2$ flakes with lateral sizes less than 100 nm. By fitting experimental data to a Ginzburg-Landau model, we estimate a zero-temperature correlation length of 10--50 nm, which matches the reported CDW domain size for 1T-TiSe$_2$. As the flake size approaches the correlation length, the divergence of the CDW correlation length near the transition is cut off by the finite flake size, limiting long-range order and thereby lowering the transition temperature. For very small flakes whose size is close to the correlation length, we also observe absence of CDWs, as predicted by the model. We thus show that an electronic phase transition follows classical nucleation theory.

cond-mat.mtrl-sci↗

arXiv2025

Liquid Helium Cryogenic TEM below 1 Å

Next-generation cryogenic transmission electron microscopes (TEM) aim to achieve high-resolution imaging at ultracold sample temperatures (< 90 K) and over extended hold times. Lower temperatures enable atomic-scale characterization with improved beam and dose resilience for organic specimens and access to emergent electronic phases in quantum materials. Side-entry liquid helium cooling stages presently lack the mechanical and thermal stability required to support sub-Angstrom information transfer in modern TEM. Here we demonstrate sub-Angstrom atomic imaging TEM with a side-entry stage at specimen temperatures down to ~20K and with low stage drift and stable hold times.

physics.ins-det↗

arXiv2025

Chiral quantum magnets with optically and catalytically active spin ladders

Chiral quantum magnets with spin-states separated by a large energy gap are technologically attractive but difficult to realize. Geometrically frustrated topological states with nanoscale chirality may offer a chemical pathway to such materials. However, room temperature spin misalignment, weakness of Dzyaloshinskii-Moriya interactions, and high energy requirements for lattice distortions set high physicochemical barriers for their realization. Here, we show that layered iron oxyhydroxides (LIOX) address these challenges due to chirality transfer from surface ligands into spin-states of dimerized FeO6 octahedra with zig-zag stacking. The intercalation of chiral amino acids induces angular displacements in the antiferromagnetic spin pairs with a helical coupling of magnetic moments along the screw axis of the zig-zag chains, or helical spin-ladders. Unlike other chiral magnets, the spin states in LIOX are chemically and optically accessible, they display strong optical resonances with helicity-matching photons and enable spin-selective charge transport. The static rather than dynamic polarization of spin ladders in LIOX makes them particularly suitable for catalysis. Room-temperature spin pairing, field-tunability, environmental robustness, and synthetic simplicity make LIOX and its intercalates a uniquely practical family of quantum magnets.

cond-mat.mtrl-sci↗

arXiv2025

Quantitative approaches for multi-scale structural analysis with atomic resolution electron microscopy

Atomic-resolution imaging with scanning transmission electron microscopy is a powerful tool for characterizing the nanoscale structure of materials, in particular features such as defects, local strains, and symmetry-breaking distortions. In addition to advanced instrumentation, the effectiveness of the technique depends on computational image analysis to extract meaningful features from complex datasets recorded in experiments, which can be complicated by the presence of noise and artifacts, small or overlapping features, and the need to scale analysis over large representative areas. Here, we present image analysis approaches which synergize real and reciprocal space information to efficiently and reliably obtain meaningful structural information with picometer scale precision across hundreds of nanometers of material from atomic-resolution electron microscope images. Damping superstructure peaks in reciprocal space allows symmetry-breaking structural distortions to be disentangled from other sources of inhomogeneity and measured with high precision. Real space fitting of the wave-like signals resulting from Fourier filtering enables absolute quantification of lattice parameter variations and strain, as well as the uncertainty associated with these measurements. Implementations of these algorithms are made available as an open source Python package.

cond-mat.mtrl-sci↗

arXiv2025

Tunable symmetry breaking in a hexagonal-stacked moiré magnet

Symmetry plays a central role in defining magnetic phases, making tunable symmetry breaking across magnetic transitions highly desirable for discovering non-trivial magnetism. Magnetic moiré superlattices, formed by twisting two-dimensional (2D) magnetic crystals, have been theoretically proposed and experimentally explored as platforms for unconventional magnetic states. However, despite recent advances, tuning symmetry breaking in moiré magnetism remains limited, as twisted 2D magnets, such as rhombohedral (R)-stacked twisted CrI_3, largely inherit the magnetic properties and symmetries of their constituent layers. Here, in hexagonal-stacked twisted double bilayer (H-tDB) CrI_3, we demonstrate clear symmetry evolution as the twist angle increases from 180^{\circ} to 190^{\circ}. While the net magnetization remains zero across this twist angle range, the magnetic phase breaks only the three-fold rotational symmetry at 180^{\circ}, but it breaks all of the rotational, mirror, and time-reversal symmetries at intermediate twist angles between 181^{\circ} and 185^{\circ}, and all broken symmetries are recovered at 190^{\circ}. These pronounced symmetry breakings at intermediate twist angles are accompanied by metamagnetic behaviors, evidenced by symmetric double hysteresis loops around zero magnetic field. Together, these results reveal that H-tDB CrI_3 at intermediate twist angles host a distinct moiré magnetic phase, featuring periodic in-plane spin textures with broken rotational, mirror, and time-reversal symmetries, which is markedly different from the out-of-plane layered antiferromagnetism in bilayer CrI_3 and the predominantly out-of-plane moiré magnetism in R-tDB CrI_3. Our work establishes H-stacked CrI_3 moiré magnets as a versatile platform for engineering magnetic properties, including and likely beyond complex spin textures.

cond-mat.mtrl-sci↗

arXiv2025

Melting of Charge Density Waves in Low Dimensions

Charge density waves (CDWs) are collective electronic states that can reshape and melt, even while confined within a rigid atomic crystal. In two dimensions, melting is predicted to be distinct, proceeding through partially ordered nematic and hexatic states that are neither liquid nor crystal. Here we measure and explain how continuous, hexatic melting of incommensurate CDWs occurs in low-dimensional materials. As a CDW is thermally excited, disorder emerges progressively$\unicode{x2013}$initially through smooth elastic deformations that modulate the local wavelength, and subsequently via the nucleation of topological defects. Experimentally, we track three hallmark signatures of CDW melting$\unicode{x2013}$azimuthal superlattice peak broadening, wavevector contraction, and integrated intensity decay.

cond-mat.mtrl-sci↗

arXiv2025

Visualizing Field-free Deterministic Magnetic Switching of all-van der Waals Spin-Orbit Torque System Using Spin Ensembles in Hexagonal Boron Nitride

Recently, optically active spin defects embedded in van der Waals (vdW) crystals have emerged as a transformative quantum sensing platform to explore cutting-edge materials science and quantum physics. Taking advantage of excellent solid-state integrability, this new class of spin defects can be arranged in controllable nanoscale proximity of target materials in vdW heterostructures, showing great promise for improving spatial resolution and field sensitivity of current sensing technologies. Building on this state-of-the-art measurement platform, here we report hexagonal boron nitride-based quantum imaging of field-free deterministic magnetic switching of room-temperature two-dimensional magnet Fe3GaTe2 in an all-vdW spin-orbit torque (SOT) system. By visualizing SOT-driven variations of nanoscale Fe3GaTe2 magnetic stray field profile under different conditions, we have revealed how the observed magnetic switching evolves from deterministic to indeterministic behavior due to the interplay between out-of-plane spins, in-plane spins and Joule heating. This understanding, which is otherwise difficult to access by conventional transport measurements, offers valuable insights on material design, testing, and evaluation of next-generation vdW spintronic devices.

cond-mat.mes-hall↗

arXiv2024

Elastic plate basis for the deformation and electron diffraction of twisted bilayer graphene on a substrate

A basis is derived from elastic plate theory that quantifies equilibrium and dynamic deformation and electron diffraction patterns of twisted bilayer graphene (TBG). The basis is derived by solving in-plane and out-of-plane normal modes of an unforced parallelogram elastic plate. We show that a combination of only a few basis terms successfully captures the relaxed TBG structure with and without an underlying substrate computed using atomistic simulations. The results are validated by comparison with electron diffraction experiments. A code for extracting the elastic plate basis coefficients from an experimental electron diffraction image accompanies this paper. TBG dynamics are also studied by computing the phonon band structure from atomistic simulations. Low-energy phonons at the $Γ$ point are examined in terms of the mode shape and frequency. These modes are captured by simple elastic plate models with uniformly distributed springs for inter-layer and substrate interactions.

cond-mat.mtrl-sci↗

arXiv2024

Imaging 3D Chemistry at 1 nm Resolution with Fused Multi-Modal Electron Tomography

Measuring the three-dimensional (3D) distribution of chemistry in nanoscale matter is a longstanding challenge for metrological science. The inelastic scattering events required for 3D chemical imaging are too rare, requiring high beam exposure that destroys the specimen before an experiment completes. Even larger doses are required to achieve high resolution. Thus, chemical mapping in 3D has been unachievable except at lower resolution with the most radiation-hard materials. Here, high-resolution 3D chemical imaging is achieved near or below one nanometer resolution in a Au-Fe$_3$O$_4$ metamaterial, Co$_3$O$_4$ - Mn$_3$O$_4$ core-shell nanocrystals, and ZnS-Cu$_{0.64}$S$_{0.36}$ nanomaterial using fused multi-modal electron tomography. Multi-modal data fusion enables high-resolution chemical tomography often with 99\% less dose by linking information encoded within both elastic (HAADF) and inelastic (EDX / EELS) signals. Now sub-nanometer 3D resolution of chemistry is measurable for a broad class of geometrically and compositionally complex materials.

physics.comp-ph↗

arXiv2024

Observation of stacking engineered magnetic phase transitions within moiré supercells of twisted van der Waals magnets

Twist engineering of magnetic van der Waals (vdW) moiré superlattices provides an attractive way to achieve precise nanoscale control over the spin degree of freedom on two-dimensional flatland. Despite the very recent demonstrations of moiré magnetism featuring exotic phases with noncollinear spin order in twisted vdW magnet chromium triiodide CrI3, the local magnetic interactions, spin dynamics, and magnetic phase transitions within and across individual moiré supercells remain elusive. Taking advantage of a scanning single-spin magnetometry platform, here we report observation of two distinct magnetic phase transitions with separate critical temperatures within a moiré supercell of small-angle twisted double trilayer CrI3. By measuring temperature dependent spin fluctuations at the coexisting ferromagnetic and antiferromagnetic regions in twisted CrI3, we explicitly show that the Curie temperature of the ferromagnetic state is higher than the Néel temperature of the antiferromagnetic one by ~10 K. Our mean-field calculations attribute such a spatial and thermodynamic phase separation to the stacking order modulated interlayer exchange coupling at the twisted interface of the moiré superlattices. The presented results highlight twist engineering as a promising tuning knob to realize on-demand control of not only the nanoscale spin order of moiré quantum matter but also its dynamic magnetic responses, which may find relevant applications in developing transformative vdW electronic and magnetic devices.

cond-mat.mes-hall↗

arXiv2024

Ultra-Cold Cryogenic TEM with Liquid Helium and High Stability

Cryogenic transmission electron microscopy has revolutionized structural biology and materials science, but achieving temperatures below the boiling point of liquid nitrogen remains a long-standing aspiration. We introduce an ultra-cold liquid helium transmission electron microscope specimen holder, featuring continuous cryogen flow and vibration decoupling. This instrument is compatible with modern aberration-corrected microscopes and achieves sub-25 K base temperature, ${\pm}$2 mK thermal stability over many hours, and atomic resolution--setting the stage for a new era of cryogenic electron microscopy.

physics.app-ph↗

arXiv2023

Imaging Atomic-Scale Chemistry from Fused Multi-Modal Electron Microscopy

Efforts to map atomic-scale chemistry at low doses with minimal noise using electron microscopes are fundamentally limited by inelastic interactions. Here, fused multi-modal electron microscopy offers high signal-to-noise ratio (SNR) recovery of material chemistry at nano- and atomic- resolution by coupling correlated information encoded within both elastic scattering (high-angle annular dark field (HAADF)) and inelastic spectroscopic signals (electron energy loss (EELS) or energy-dispersive x-ray (EDX)). By linking these simultaneously acquired signals, or modalities, the chemical distribution within nanomaterials can be imaged at significantly lower doses with existing detector hardware. In many cases, the dose requirements can be reduced by over one order of magnitude. This high SNR recovery of chemistry is tested against simulated and experimental atomic resolution data of heterogeneous nanomaterials.

physics.comp-ph↗