arXiv subjects

Eric A. Stach

Publications and source records attributed to Eric A. Stach.

At least 19 recordsLinked to original sources

arXiv2026

Compositional gradient engineering for enhanced ferroelectricity in ultrathin AlScN

Ferroelectric AlScN is promising for CMOS-compatible non-volatile memory, but thickness scaling is limited by leakage, premature breakdown, and defect-mediated failure. Here we show that compositional grading within a continuous wurtzite AlN-AlScN lattice mitigates these limitations by distributing structural and polarization discontinuities across the film thickness, reducing defect formation and local field concentration. In a 20 nm graded heterostructure, monotonic Sc incorporation and AlN-rich boundaries produce reversible ferroelectric switching, an as-grown metal-polar state, a 21% higher breakdown field, 10% enhanced remanent polarization, and 40x higher resistivity relative to homogeneous AlScN. Time-domain PUND measurements reveal strongly suppressed post-switching leakage, consistent with reduced defect-assisted and polarization-coupled conduction. This improved dielectric robustness enables ferroelectric functionality in 5 nm graded stacks containing only a 2 nm $\mathrm{Al}_{0.64}\mathrm{Sc}_{0.36}\mathrm{N}$ region, with measurable switching near 1 V. These results establish compositional grading as a defect- and field-management strategy for scalable ultrathin wurtzite ferroelectrics.

cond-mat.mtrl-sci↗

arXiv2026

Crystallizing Substrates Drag Supported Nanoparticles

When a solid support undergoes crystallization, the advancing amorphous-to-crystalline transformation front separates regions of distinct surface energy, creating a moving interfacial energy boundary. A supported nanoparticle straddling such a boundary experiences an asymmetric particle-substrate interfacial energy environment that constitutes a lateral thermodynamic driving force for migration. Here, using in situ transmission electron microscopy to track Pt nanoparticle motion statistically, paired with time-resolved diffraction and 4D-STEM analysis to characterize support crystallization, we demonstrate that propagating crystallization fronts in amorphous AlO$_x$ thin films actively drag supported Pt nanoparticles over long distances. Temporal correlation between the onsets of support crystallization and rapid particle migration, together with 4D-STEM virtual crystallinity maps, establishes that the front drives particle motion. Phase-field simulations confirm that particle-substrate interfacial energy contrast alone sustains particle drag, and identify curvature gradients along the particle surface as the mechanism by which the advancing front redistributes mass and displaces the particle. These results establish a general mechanism by which any propagating surface-energy boundary on a substrate can act as a deterministic driver of supported nanoparticle transport.

cond-mat.mtrl-sci↗

arXiv2026

Substrate-Mediated Evaporation and Stochastic Evolution of Supported Au Nanoparticles

We use in situ transmission electron microscopy with automated tracking to study supported gold nanoparticles (NPs) during high-temperature vacuum annealing. \rev{The average mass loss per NP is governed by a flat, nearly size-independent substrate-mediated evaporation profile.} On top of \rev{this mean shrinkage}, individual NPs show significant fluctuations in apparent growth or shrinkage, and NP volume follows a \rev{random-walk-like trajectory. To rationalize both the ensemble-mean behavior and the particle-resolved variability, we develop a self-consistent theory that couples substrate-mediated evaporation to collective 2D Ostwald-type mass exchange through a shared adatom field, described in terms of a renormalized screening length and background concentration. In the experimentally relevant regime, the theory predicts an approximately size-independent mean shrinkage rate and clarifies how net mass loss suppresses classical coarsening.} \rev{Superimposed on this deterministic drift, we quantify stochastic volume trajectories and capture their fluctuation spectrum with a minimal Langevin description consistent with intermittent adatom attachment and detachment events.} In addition, we characterize the lateral diffusive motion of NPs, which is responsible for their coalescence. Altogether, our results highlight that stochasticity is intrinsic at the nanoscale \rev{and that predicting the evolution of supported NPs at early and intermediate times requires a unified framework combining substrate-mediated evaporation, collective mass exchange, and stochastic fluctuations.

cond-mat.mtrl-sci↗

arXiv2026

Probing Plasmonic Oscillations in 2D Moir\'e Nanocrystal Superlattices by Low-Loss EELS

Electron energy loss spectroscopy (EELS) has been established as a powerful analytical technique for investigating the oxidation state, band structure, and dielectric properties of materials with exceptional spatial resolution. Inspired by twisted 2D materials, we utilize low-loss EELS to examine the plasmonic excitations in 2D moir\'e Au nanocrystal superlattices (NCSLs) formed by liquid-air interface self-assembly using a double-dipping method. This approach produces stacked hexagonal layers that can be twisted, forming moir\'e patterns in NCSLs whose twist angles are precisely measured via scanning transmission electron microscopy (STEM). Low-loss EELS effectively mitigates challenges arising from fabrication-induced non-uniformity and reveals a blue shift in plasmonic excitation when comparing single-layer, double-layer, and twisted configurations. This sharply contrasts with the optical spectroscopy measurements, which show an overall red shift relative to the EELS data. The high spatial resolution of STEM-EELS further demonstrates that twist-induced symmetry breaking strongly influences plasmonic behavior. Coupled dipole modeling explains the observed discrepancies: the electron beam excites out-of-plane polarization modes unavailable to optical probes, while optical measurements average over ensembles. Our findings highlight that EELS provides complementary information to optical spectroscopy for understanding how structural arrangements at the nanoscale influence collective electronic properties, advancing the design of plasmonic metamaterials.

cond-mat.mtrl-sci↗

arXiv2025

Tuning Breakdown-to-Coercive Field Ratio in Ultra-Thin Al1-xScxN Films via Reactive Nitrogen Atmosphere

Al1-xScxN has attracted significant interest due to its large remnant polarization and low processing temperature when compared to other ferroelectric material systems. However, device dielectric failure before ferroelectric switching remains a critical limitation for AlScN-based memory devices. With the continuing trend toward device miniaturization, expanding the operating window is essential for next-generation memory development. In this work, we optimized the breakdown field (EBD) and coercive field (EC) in ultra-thin Al1-xScxN films by controlling defect density via adjustment of nitrogen gas flow during sputter deposition. The characteristic breakdown field, EBD, was evaluated using Weibull statistics, yielding optimal characteristic breakdown fields of 12.47 MV/cm (EBD+) and -12.63 MV/cm (EBD-) for samples deposited under 27.5 sccm N2 flow. The minimum EC was achieved at a nitrogen flow of 25 sccm and increased for higher gas flows, a trend that is opposite to previous reports in much thicker films. The highest EBD over EC ratio of 2.25 occurred at 27.5 sccm, effectively expanding the operational window. Using a combination of X-ray diffraction and photoluminescence spectroscopy to study changes in crystal orientation and defects, device performance can be tuned by controlling the point defect concentration in the ultra-thin film via adjusting the sputtering N2 process gas flow rate.

cond-mat.mtrl-sci↗

arXiv2025

Low-Field Ferroelectricity in 10 nm AlBScN Thin Films

Ferroelectric aluminum scandium nitride (Al1-xScxN, AlScN) offers CMOS-compatible integration but suffers from high coercive fields and leakage currents that hinder thickness scaling. Further reduction in thickness is essential for low-voltage embedded nonvolatile memory applications. Boron incorporation into AlScN (AlBScN) suppresses leakage current in films down to 40 nm, yet its ferroelectric characteristics in ultrathin films remains unexplored. This letter demonstrates robust ferroelectric switching in 10 nm sputtered AlBScN capacitors with a low coercive field and approximately two orders of magnitude lower leakage than AlScN. Notably, ferroelectric switching was observed at 2.2 MV/cm in capacitance-voltage measurements, and symmetric polarization reversal occurred near 4.6 MV/cm in positive-up-negative-down (PUND) measurements using 2 {\mu}s pulses. Moreover, Weibull analysis revealed a breakdown-to-coercive-field ratio (EBD/Ec) of ~2.2. These findings demonstrated AlBScN as a promising candidate for CMOS back-end-of-line (BEOL) compatible ferroelectric applications with improved energy consumption and reduced leakage current.

cond-mat.mtrl-sci↗

arXiv2025

Evolution of electronic and magnetic properties in Mn- and Co-alloyed ferromagnetic kagome metal Fe3Sn2

Kagome metals are an intriguing class of quantum materials as the presence of both flat bands and Dirac points provides access to functional properties present in strongly correlated and topological materials. To fully harness these electronic features, the ability to tune the Fermi level relative to the band positions is needed. Here we explore the structural, electronic and magnetic impacts of substitutional alloying within ferromagnetic kagome metal Fe3Sn2 in thin films grown by molecular beam epitaxy. Transition metals Mn and Co are chosen as substitutes for Fe to reduce or increase the d-band electron count, thereby moving the Fermi level accordingly. We find that Co is not incorporated into the Fe3Sn2 structure but instead results in a two-phase Fe-Co and (Fe,Co)Sn composite. In contrast, Fe3-xMnxSn2 films are realized with x up to 1.0, retaining crystalline quality comparable to the parent phase. The incorporation of Mn repositions the flat bands relative to the Fermi level in a manner consistent with hole-doping, as revealed by hard x-ray photoemission and density functional theory. The Fe3-xMnxSn2 films retain room temperature ferromagnetism, with x-ray magnetic circular dichroism measurements confirming that the Fe and Mn moments are ferromagnetically aligned. The ability to hole-dope this magnetic kagome metal provides a platform for tuning properties such as anomalous Hall and Nernst responses.

cond-mat.mtrl-sci↗

arXiv2025

Coercive Field Reduction in Ultra-thin Al1-XScXN via Interfacial Engineering with a Scandium Electrode

Aluminum scandium nitride (AlScN) ferroelectrics are promising for next-generation non-volatile memory applications due to high remnant polarization compared with Pb(ZrxTi1-x)O3 and doped-HfO2 material systems, as well as their fast switching and scalability to nanometer thicknesses. As AlScN films are thinned to 10 nm thickness, coercive field has been shown to substantially increase, which hinders low voltage operation. We demonstrate that interfacial engineering through bottom electrode selection and strain management reduces this coercive field increase with scaling and improves ferroelectric performance. Here, we demonstrate robust ferroelectricity in ultra-thin AlScN capacitors deposited on a Sc bottom electrode under both alternating current and direct current conditions. The coercive field is reduced by over 20 percent compared to capacitors with an Al bottom electrode. Furthermore, the difference in dynamic switching behavior over a decade of frequency was evaluated by applying the KAI model. At frequencies lower than 16.7 kHz, the capacitors with Sc and Al bottom electrodes exhibit comparable KAI exponents of 0.030 and 0.028, indicating similar switching kinetics. However, at higher frequencies, the capacitor with an Al bottom electrode shows a significantly higher exponent of 0.063, indicating a stronger frequency dependence, whereas the capacitor with a Sc bottom electrode maintains a stable exponent of 0.030, suggesting a lower frequency dependence during faster switching scenarios. The Scanning Electron Nanobeam Diffraction technique was selected to measure the strain difference in AlScN thin films grown on templates with different lattice mismatch, providing a correlation between lattice mismatch, film strain and switching behavior in ultra-thin film systems.

cond-mat.mtrl-sci↗

arXiv2025

Demonstration of highly scaled AlScN ferroelectric diode memory with storage density > 100 Mbit/mm$^2$

Wurtzite nitride ferroelectric materials have emerged as promising candidates for next-generation memory applications due to their exceptional polarization properties and compatibility with conventional semiconductor processing techniques. Here, we demonstrate the first successful areal scaling of Aluminum Scandium Nitride (AlScN) ferroelectric diode (FeDiode) memory down to 40 nm device diameters while maintaining ON/OFF > 60. Using a 20 nm thick Al0.64Sc0.36N ferroelectric layer, we evaluate both metal-insulator-ferroelectric-metal (MIFM) and metal-ferroelectric-metal (MFM) architectures for scaled resistive memory devices. Our scaled devices exhibit an enhanced breakdown-to-coercive field ratio exceeding 2.6 due to increased breakdown field. The MIFM devices demonstrate stable 3-bit non-volatile multistate behavior with clearly distinguishable resistance states and retention exceeding 4*10^4 seconds at 85 C. By achieving more than a million-fold areal scaling with enhanced performance metrics, this work establishes AlScN-based FeDiode memory as a highly promising platform for non-volatile storage with potential for direct integration into CMOS technology.

cond-mat.mes-hall↗

arXiv2025

Hydrazine-Free Precursor for Solution-Processed All-Inorganic Se and Se1-xTex Photovoltaics

Selenium (Se) has reemerged as a promising absorber material for indoor and tandem photovoltaics (PVs), and its alloys with Te (Se1-xTex) offer a widely tunable bandgap. Solution processing of this materials system offers a route to low-cost fabrication. However, solution processing of Se has, thus far, only used hydrazine, which is an extremely hazardous solvent. In this work, we prepare and isolate propylammonium poly-Se and poly-Se-Te precursors from a safer thiol-amine solvent system. We formulate molecular inks by dissolving the precursor n,n-dimethylformamide (DMF) with a monoethanolamine (EA) additive and process high-quality Se and Se1-xTex films with bandgaps ranging from 1.20 eV to 1.86 eV. We fabricate PVs from these films using TiO2 and MoO3 charge transport layers (CTLs) to achieve power conversion efficiencies as high as 2.73% for Se and 2.33% for Se0.7Te0.3 under solar simulation. Se devices show excellent stability with no degradation after 1 month in air, enabled by the excellent stability of Se and the use of inorganic CTLs. This work represents an important step towards low-cost solution-phase processing of Se and Se1-xTex alloys for PVs and photodetectors with low toxicity and high bandgap tunability.

cond-mat.mtrl-sci↗

arXiv2025

Interfacial Energy Gradients Drive Coalescence of Supported Nanoparticles

Understanding and controlling nanoparticle coalescence is crucial for applications ranging from catalysis to nanodevice fabrication, yet the behavior of nanoparticles on dynamically evolving, heterogeneous substrates remains poorly understood. Here, we employ in situ transmission electron microscopy to investigate platinum (Pt) nanoparticle dynamics on silicon nitride (SiN$_x$) substrates where localized crystalline silicon (Si) nanodomains are deliberately formed via electron beam irradiation at $800^\circ$C. We observe that Pt nanoparticles in contact with these Si pads transform into a more mobile platinum silicide (Pt$_3$Si) phase. Strikingly, these Pt$_3$Si nanoparticles exhibit pronounced directional migration away from the Si pads, driven by interfacial energy gradients, rather than undergoing stochastic Brownian motion. This directed movement fundamentally dictates coalescence pathways, leading to either enhanced sintering when particles are channeled together or inhibited coalescence when Si pads act as repulsive barriers. Our findings reveal that local substrate chemistry and the resulting interfacial energy landscapes can dominate over initial particle size or proximity in controlling solid-state nanoparticle migration and assembly. This work provides insights into how substrate heterogeneity can be used to direct nanoparticle behavior, challenging conventional coalescence models and offering pathways for the rational design of supported nanomaterials.

cond-mat.mtrl-sci↗

arXiv2025

Observation of Order and Disorder in Solid-Electrolyte Interphases of Lithium-Metal Anodes

Battery interfaces critically influence lithium-metal battery performance through their role in ion diffusion and dendrite formation. However, structural characterization of these interfaces has remained challenging due to limitations in high-resolution methods and artifacts from electron irradiation. Using cryogenic conditions for both specimen preparation and scanning electron nanobeam diffraction, we can determine the structural organization at the interface between the vitrified electrolyte and adjacent layers. We identified two distinct interface types: one showing short-range order adjacent to lithium metal, and another displaying a mixed structure of short-range ordering and defective lithium fluoride nanoscale crystallites at a copper collector. Notably, short-range order appeared exclusively in electrolytes demonstrating high reversibility. Our results establish that solid-electrolyte-interphase structure directly influences lithium deposition morphology and battery performance. This methodology opens new possibilities for high-resolution characterization of interfaces in energy storage materials, advancing our understanding of their critical structural properties.

cond-mat.mtrl-sci↗

arXiv2024

Reconfigurable Compute-In-Memory on Field-Programmable Ferroelectric Diodes

The deluge of sensors and data generating devices has driven a paradigm shift in modern computing from arithmetic-logic centric to data-centric processing. Data-centric processing require innovations at device level to enable novel compute-in-memory (CIM) operations. A key challenge in construction of CIM architectures is the conflicting trade-off between the performance and their flexibility for various essential data operations. Here, we present a transistor-free CIM architecture that permits storage, search and neural network operations on sub-50nm thick Aluminum Scandium Nitride ferroelectric diodes (FeDs). Our circuit designs and devices can be directly integrated on top of Silicon microprocessors in a scalable process. By leveraging the field-programmability, non-volatility and non-linearity of FeDs, search operations are demonstrated with a cell footprint < 0.12 um2 when projected onto 45-nm node technology. We further demonstrate neural network operations with 4-bit operation using FeDs. Our results highlight FeDs as candidates for efficient and multifunctional CIM platforms.

physics.app-ph↗

arXiv2024

Giant Optical Anisotropy in 2D Metal-Organic Chalcogenates

Optical anisotropy is a fundamental attribute of some crystalline materials and is quantified via birefringence. A birefringent crystal not only gives rise to asymmetrical light propagation but also attenuation along two distinct polarizations, a phenomenon called linear dichroism (LD). Two-dimensional (2D) layered materials with high in- and out-of-plane anisotropy have garnered interest in this regard. Mithrene, a 2D metal-organic chalcogenate (MOCHA) compound, exhibits strong excitonic resonances due to its naturally occurring multi-quantum well (MQW) structure and in-plane anisotropic response in the blue wavelength (~400-500 nm) regime. The MQW structure and the large refractive indices of mithrene allow the hybridization of the excitons with photons to form self-hybridized exciton-polaritons in mithrene crystals with appropriate thicknesses. Here, we report the giant birefringence (~1.01) and tunable in-plane anisotropic response of mithrene, which stem from its low symmetry crystal structure and unique excitonic properties. We show that the LD in mithrene can be tuned by leveraging the anisotropic exciton-polariton formation via the cavity coupling effect exhibiting giant in-plane LD (~77.1%) at room temperature. Our results indicate that mithrene is an ideal polaritonic birefringent material for polarization-sensitive nanophotonic applications in the short wavelength regime.

physics.optics↗

arXiv2024

Multi-State, Ultra-thin, BEOL-Compatible AlScN Ferroelectric Diodes

The growth in data generation necessitates efficient data processing technologies to address the von Neumann bottleneck in conventional computer architecture. Memory-driven computing, which integrates non-volatile memory (NVM) devices in a 3D stack, is gaining attention, with CMOS back-end-of-line (BEOL) compatible ferroelectric (FE) diodes being ideal due to their two-terminal design and inherently selector-free nature, facilitating high-density crossbar arrays. Here, we demonstrate BEOL-compatible, high-performance FE-diodes scaled to 5, 10, and 20 nm FE Al0.72Sc0.28N/Al0.64Sc0.36N films. Through interlayer (IL) engineering, we show substantial improvements in the ON/OFF ratios (>166 times) and rectification ratios (>176 times) in these scaled devices. The superlative characteristics also enables 5-bit multi-state operation with a stable retention. We also experimentally and theoretically demonstrate the counterintuitive result that the inclusion of an IL can lead to a decrease in the ferroelectric switching voltage of the device. An in-depth analysis into the device transport mechanisms is performed, and our compact model aligns seamlessly with the experimental results. Our results suggest the possibility of using scaled AlxSc1-xN FE-diodes for high performance, low-power, embedded NVM.

cond-mat.mtrl-sci↗

arXiv2024

Epitaxial growth and magnetic properties of kagome metal FeSn/elemental ferromagnet heterostructures

Binary kagome compounds TmXn (T = Mn, Fe, Co; X = Sn, Ge; m:n = 3:1, 3:2, 1:1) have garnered recent interest owing to the presence of both topological band crossings and flat bands arising from the geometry of the metal-site kagome lattice. To exploit these electronic features for potential applications in spintronics, the growth of high quality heterostructures is required. Here we report the synthesis of Fe/FeSn and Co/FeSn bilayers on Al2O3 substrates using molecular beam epitaxy to realize heterointerfaces between elemental ferromagnetic metals and antiferromagnetic kagome metals. Structural characterization using high-resolution X-ray diffraction, reflection high-energy electron diffraction, and electron microscopy reveals the FeSn films are flat and epitaxial. Rutherford backscattering spectroscopy was used to confirm the stoichiometric window where the FeSn phase is stabilized, while transport and magnetometry measurements were conducted to verify metallicity and magnetic ordering in the films. Exchange bias was observed, confirming the presence of antiferromagnetic order in the FeSn layers, paving the way for future studies of magnetism in kagome heterostructures and potential integration of these materials into devices.

cond-mat.mtrl-sci↗

arXiv2023

Scalable and Stable Ferroelectric Non-Volatile Memory at > 500 $^\circ$C

Non-volatile memory (NVM) devices that reliably operate at temperatures above 300 $^\circ$C are currently non-existent and remains a critically unmet challenge in the development of high-temperature (T) resilient electronics, necessary for many emerging, complex computing and sensing in harsh environments. Ferroelectric Al$_x$Sc$_{1-x}$N exhibits strong potential for utilization in NVM devices operating at very high temperatures (> 500 $^\circ$C) given its stable and high remnant polarization (PR) above 100 $μ$C/cm$^2$ with demonstrated ferroelectric transition temperature (TC) > 1000 $^\circ$C. Here, we demonstrate an Al$_{0.68}$Sc$_{0.32}$N ferroelectric diode based NVM device that can reliably operate with clear ferroelectric switching up to 600 $^\circ$C with distinguishable On and Off states. The coercive field (EC) from the Pulsed I-V measurements is found to be -5.84 (EC-) and +5.98 (EC+) (+/- 0.1) MV/cm at room temperature (RT) and found to decrease with increasing temperature up to 600 $^\circ$C. The devices exhibit high remnant polarizations (> 100 $μ$C/cm$^2$) which are stable at high temperatures. At 500 $^\circ$C, our devices show 1 million read cycles and stable On-Off ratio above 1 for > 6 hours. Finally, the operating voltages of our AlScN ferrodiodes are < 15 V at 600 $^\circ$C which is well matched and compatible with Silicon Carbide (SiC) based high temperature logic technology, thereby making our demonstration a major step towards commercialization of NVM integrated high-T computers.

physics.app-ph↗

arXiv2023

Ultra-fast Vacancy Migration: A Novel Approach for Synthesizing Sub-10 nm Crystalline Transition Metal Dichalcogenide Nanocrystals

Two-dimensional materials, such as transition metal dichalcogenides (TMDCs), have the potential to revolutionize the field of electronics and photonics due to their unique physical and structural properties. This research presents a novel method for synthesizing crystalline TMDCs crystals with < 10 nm size using ultra-fast migration of vacancies at elevated temperatures. Through in-situ and ex-situ processing and using atomic-level characterization techniques, we analyze the shape, size, crystallinity, composition, and strain distribution of these nanocrystals. These nanocrystals exhibit electronic structure signatures that differ from the 2D bulk i.e., uniform mono and multilayers. Further, our in-situ, vacuum-based synthesis technique allows observation and comparison of defect and phase evolution in these crystals formed under van der Waals heterostructure confinement versus unconfined conditions. Overall, this research demonstrates a solid-state route to synthesizing uniform nanocrystals of TMDCs and lays the foundation for materials science in confined 2D spaces under extreme conditions.

cond-mat.mtrl-sci↗