arXiv subjects

Pinshane Y. Huang

Publications and source records attributed to Pinshane Y. Huang.

At least 19 recordsLinked to original sources

arXiv2026

PtyRANNOSAUR: Ptychography with Robust Artificial Neural Networks Optimized for Sub-Angstrom Accuracy and Ultrafast Reconstruction

We present PtyRANNOSAUR, a data-driven neural network code that reconstructs atomic resolution electron ptychography data in seconds, 10-100x faster than standard methods. PtyRANNOSAUR uses convolutional autoencoders to map 4D-scanning transmission electron microscopy data to 2D phase images. Each model is trained on a large database of crystal structures and is tailored for a range of experimental parameters, such as accelerating voltage, convergence angle, defocus, and sample thickness. This approach yields high quality reconstructions without requiring any fine-tuning of hyperparameters. In addition, the code handles spatial partial coherence, multiple scattering, and scan position errors, which are critical for state-of-the-art electron ptychography reconstructions. By testing PtyRANNOSAUR on experimental and simulated data, we show that the neural networks accurately reconstruct atomic structures of a broad range of materials systems and can achieve high resolutions of $<0.5$ Å, comparable to the best iterative reconstructions of the same data. These advances enable near-live, state-of-the-art electron ptychography reconstructions.

cond-mat.mtrl-sci↗

arXiv2026

Millimeter-Scale, Atomically Controlled 2D Topological Insulators Revealed by Multimodal Spectroscopy

Quantum spin Hall insulators, or synonymously known as 2D topological insulators, are crucial 2D systems hosting topologically protected edge states. The working temperature of this topological quantum phase is dictated by the inverted bandgap. However, the previously identified large-gap 2D topological insulators are either extremely chemically unstable, or cannot be made with atomistic precision over macroscopic scales. Here, we establish two-quintuple-layer Bi2Te3 and MnBi2Te4/Bi2Te3 heterostructures as atomically controlled, millimeter-scale 2D topological insulators, enabled by precision layer-by-layer growth that yields a carpet-like morphology extending coherently over macroscopic distances. This carpet-like growth mode renders the films amenable to mechanical exfoliation and subsequent wet or dry transfer. Multimodal spectroscopies and microscopies reveal the integer-layer tuned electronic structure of (Bi2Te3)n with excellent agreement to theory. Photon-energy-dependent photoemission and time-resolved photoemission identify band inversion and band dynamics, respectively, while scanning tunneling spectroscopy resolves topological edge states, characteristic of the 2D topological insulator phase. Thickness- and photon-energy-dependent photoemission further validates MnBi2Te4/Bi2Te3 as a robust 2D topological insulator. The large inverted gaps of ~100 meV in (Bi2Te3)2 and ~150 meV in MnBi2Te4/Bi2Te3 suggest operation near ambient temperature. These results define a scalable materials platform for next-generation, low-loss quantum and energy-efficient devices.

cond-mat.mtrl-sci↗

arXiv2026

Structural control of two-level defect density revealed by high-throughput correlative measurements of Josephson junctions

Materials defects in Josephson junctions (JJs), often referred to as two-level systems (TLS), couple to superconducting qubits and are a critical bottleneck for scalable quantum processors. Despite their importance, understanding the microscopic sources of TLS and how to mitigate them has remained a major challenge. Here, we demonstrate a high-throughput, correlated approach to trace the microstructural origins of strongly-coupled TLS in Josephson circuits. We assembled a massive dataset of TLS across 6,000 Al/AlOx/Al JJs and more than 600 atomic resolution transmission electron microscopy images. We statistically link fabrication, microstructure, and TLS occurrence, revealing a strong correlation between Al electrode thickness, Al grain size, and TLS density. Correspondingly, we find a two-thirds reduction in TLS prompted by a change in electrode fabrication parameters. These results demonstrate a robust, data-driven methodology to understand and control defects in quantum circuits and pave the way for significantly reducing TLS density.

quant-ph↗

arXiv2026

Atomic and Electronic Structure of Strongly Charged Domain Walls in van der Waals α-In$_2$Se$_3$

Here, we use atomic resolution scanning transmission electron microscopy (STEM) and first principles calculations to study the atomic and electronic structure of strongly charged domain walls in $α$-In$_2$Se$_3$. STEM imaging and density functional theory (DFT) show that head-to-head (HH) domain walls contain a layer of nonpolar $β$-In$_2$Se$_3$, whereas tail-to-tail (TT) domain walls are atomically abrupt. We apply 4D STEM and multislice electron ptychography to map ferroelectric domains in 2D and 3D, showing that nearly $180^\circ$ domain walls exhibit complex, curved 3D structures that differ from ideal $180^\circ$ structures. Band structure calculations show localized conducting states within a $\sim$ 1 nm thick layer at both HH and TT domain walls, such as a midgap state at the $β$ layer of the HH domain wall. These properties make strongly charged domain walls in $α$-In$_2$Se$_3$ excellent candidates for realizing 2D electron or hole gases and domain wall engineering in van der Waals ferroelectrics.

cond-mat.mtrl-sci↗

arXiv2025

Enhancing Hole Mobility in Monolayer $WSe_{2}$ p-FETs via Process-Induced Compression

Understanding the interactions between strain, interfacial mechanics, and electrical performance is critical for designing beyond silicon electronics based on hetero-integrated 2D materials. Through combined experiment and simulation, we demonstrated and analyzed the enhancement of hole mobility in p-type monolayer $WSe_{2}$ field effect transistors (FETs) under biaxial compression. We tracked FET performance versus strain by incrementing compressive strain to $WSe_{2}$ channels via sequential AlOx deposition and performing intermediate photoluminescence and transport measurements. The hole mobility factor increased at a rate of 340 $\pm$ 95 %/%$ε$, and the on-current factor increased at a rate of 460 $\pm$ 340 %/%$ε$. Simulation revealed that the enhancement under compression arises primarily from a reduction in inter-valley scattering between the $Γ$--K valence bands, and the rate is robust against variations in carrier density, impurity density, or dielectric environment. These findings show that compressive strain is a powerful technique for enhancing performance in 2D p-FETs and that it is multiplicative with defect and doping engineering.

cond-mat.mtrl-sci↗

arXiv2025

3D Mapping of Defects and Moiré Corrugations via Electron Ptychography Atomic Coordinate Retrieval

Defects and reconstructions in 2D moiré materials cause out-of-plane deformations which strongly modify their electronic properties but are difficult to experimentally access. Here, we solve the 3D atomic coordinates of twisted bilayer WSe$_2$ with picometer-scale accuracy using multislice electron ptychography (MEP) acquired from a single orientation. The resulting atomic models individually visualize each of the six atomic planes, revealing the curvature of each WSe$_2$ layer, variations in the interlayer spacing, and the 3D locations of individual vacancies -- which lie exclusively in the outer Se planes. We also observe a new, unexpected type of structural disorder consisting of mixed bending -- and breathing-type moiré-induced corrugations that should strongly impact the emergent electronic properties. Broadly, our methods generate 3D atom-by-atom models of a 2D heterointerface from data acquired in about 30 seconds, methods that should unlock routine access to 3D atomic information in 2D systems and catalyze design methods to control out-of-plane deformations.

cond-mat.mtrl-sci↗

arXiv2025

Wafer-scale Programmed Assembly of One-atom-thick Crystals

Crystalline films offer various physical properties based on the modulation of their thicknesses and atomic structures. The layer-by-layer assembly of atomically thin crystals provides powerful means to arbitrarily design films at the atomic-level, which are unattainable with existing growth technologies. However, atomically-clean assembly of the materials with high scalability and reproducibility remains challenging. We report programmed crystal assembly (PCA) of graphene and monolayer hexagonal boron nitride (ML hBN), assisted by van der Waals interactions, to form wafer-scale films of pristine interfaces with near-unity yield. The atomic configurations of the films are tailored with layer-resolved compositions and in-plane crystalline orientations. We demonstrate batch-fabricated tunnel device arrays with modulation of the resistance over orders of magnitude by thickness-control of the hBN barrier with single-atom precision, and large-scale, twisted multilayer graphene with programmable electronic band structures and crystal symmetries. Our results constitute an important development in the artificial design of large-scale films.

cond-mat.mtrl-sci↗

arXiv2025

Field-effect transistors based on charged domain walls in van der Waals ferroelectric α-In$_2$Se$_3$

Charged domain walls (CDW) in ferroelectrics are emerging as functional interfaces with potential applications in nonvolatile memory, logic, and neuromorphic computing. However, CDWs in conventional ferroelectrics are vertical, buried, or electrically inaccessible interfaces that prevent their use in functional devices. Here, we overcome these challenges by stacking two opposite polar domains of van der Waals ferroelectric $α$-In$_2$Se$_3$ to generate artificial head-head (H-H) CDWs and use edge contact to fabricate charged domain wall-based field-effect transistors (CDW-FET). We relate the atomic structure to the temperature-dependent electrical and magneto-transport of the CDW-FET. CDW-FETs exhibit a metal-to-insulator transition with decreasing temperature and enhanced conductance and field-effect mobility compared to single domain $α$-In$_2$Se$_3$. We identify two regimes of transport: variable range hopping due to disorder in the band edge below 70 K and thermally activated interfacial trap-assisted transport above 70 K. The CDW-FETs show room-temperature resistance down to 3.1 k$Ω$ which is 2-9 orders of magnitude smaller than the single CDW in thin-film ferroelectrics. These results resolve longstanding challenges with high CDW resistance and their device integration, opening opportunities for gigahertz memory and neuromorphic computing.

cond-mat.mtrl-sci↗

arXiv2025

Atom-by-atom Imaging of Moiré Phasons using Electron Ptychography

Twisted 2D materials exhibit unique vibrational modes called moiré phonons, which arise from the moiré superlattice. Here, we demonstrate atom-by-atom imaging of phasons, an ultrasoft class of moiré phonons in twisted bilayer WSe2. Using ultrahigh-resolution (<15 pm) electron ptychography, we image the size and shape of each atom to extract time-averaged vibrational amplitudes as a function of twist angle and position. We observe several signature properties of moiré phasons, such as increased vibrational amplitudes at solitons and AA-stacked regions. By correlating experiments with molecular dynamics simulations and lattice dynamics calculations, we show phasons dominate the thermal vibrations in low-angle twisted bilayers. These results represent a powerful route to image thermal vibrations at atomic resolution, unlocking experimental studies of a thus-far hidden branch of moiré phonon physics.

cond-mat.mtrl-sci↗

arXiv2025

A Topological Superconductor Tuned by Electronic Correlations

A topological superconductor, characterized by either a chiral order parameter or a chiral topological surface state in proximity to bulk superconductivity, is foundational to topological quantum computing. As in other topological phases of matter, electronic correlations can tune topological superconductivity via modifications of the low-energy Fermiology. Such tuning has not been realized so far. Here we uncover a unique topological superconducting phase in competition with electronic correlations in 10-unit-cell thick FeTe$_{x}$Se$_{1-x}$ films grown on SrTiO$_{3}$ substrates. When the Te content $x$ exceeds $0.7$, we observe a rapid increase of the effective mass for the Fe $d_{xy}$ band, with the emergence of a superconducting topological surface state confirmed by high-resolution angle-resolved photoemission spectroscopy; however, near the FeTe limit, the system enters an incoherent regime where the topological surface state becomes unidentifiable and superconductivity is suppressed. Theory suggests that the electron-electron interactions in the odd-parity $xy^-$ band with a strong $d_{xy}$ character lead to an orbital-selective correlated phase. Our work establishes FeTe$_{x}$Se$_{1-x}$ thin films as a unique platform where electronic correlations sensitively modulate topological superconductivity, suggesting opportunities to use tunable electron-electron interactions to engineer new topological phases in a broad class of materials.

cond-mat.supr-con↗

arXiv2024

Disorder and diffuse scattering in single-chirality (TaSe$_4$)$_2$I crystals

The quasi-one-dimensional chiral compound (TaSe$_4$)$_2$I has been extensively studied as a prime example of a topological Weyl semimetal. Upon crossing its phase transition temperature $T_\textrm{CDW}$ $\approx$ 263 K, (TaSe$_4$)$_2$I exhibits incommensurate charge density wave (CDW) modulations described by the well-defined propagation vector $\sim$(0.05, 0.05, 0.11), oblique to the TaSe$_4$ chains. Although optical and transport properties greatly depend on chirality, there is no systematic report about chiral domain size for (TaSe$_4$)$_2$I. In this study, our single-crystal scattering refinements reveal a bulk iodine deficiency, and Flack parameter measurements on multiple crystals demonstrate that separate (TaSe$_4$)$_2$I crystals have uniform handedness, supported by direct imaging and helicity dependent THz emission spectroscopy. Our single-crystal X-ray scattering and calculated diffraction patterns identify multiple diffuse features and create a real-space picture of the temperature-dependent (TaSe$_4$)$_2$I crystal structure. The short-range diffuse features are present at room temperature and decrease in intensity as the CDW modulation develops. These transverse displacements, along with electron pinning from the iodine deficiency, help explain why (TaSe$_4$)$_2$I behaves as an electronic semiconductor at temperatures above and below $T_\textrm{CDW}$, despite a metallic band structure calculated from density functional theory of the ideal structure.

cond-mat.str-el↗

arXiv2023

Leveraging generative adversarial networks to create realistic scanning transmission electron microscopy images

The rise of automation and machine learning (ML) in electron microscopy has the potential to revolutionize materials research through autonomous data collection and processing. A significant challenge lies in developing ML models that rapidly generalize to large data sets under varying experimental conditions. We address this by employing a cycle generative adversarial network (CycleGAN) with a reciprocal space discriminator, which augments simulated data with realistic spatial frequency information. This allows the CycleGAN to generate images nearly indistinguishable from real data and provide labels for ML applications. We showcase our approach by training a fully convolutional network (FCN) to identify single atom defects in a 4.5 million atom data set, collected using automated acquisition in an aberration-corrected scanning transmission electron microscope (STEM). Our method produces adaptable FCNs that can adjust to dynamically changing experimental variables with minimal intervention, marking a crucial step towards fully autonomous harnessing of microscopy big data.

cond-mat.mtrl-sci↗

arXiv2023

In situ Imaging of an Anisotropic Layer-by-Layer Phase Transition in Few-Layer MoTe2

Understanding the phase transition mechanisms in two-dimensional (2D) materials is a key to precisely tailor their properties at the nanoscale. Molybdenum ditelluride (MoTe2) exhibits multiple phases at room temperature, making it a promising candidate for phase-change applications. Here, we fabricate lateral 2H-Td interfaces with laser irradiation and probe their phase transitions from micro- to atomic scales with in situ heating in the transmission electron microscope (TEM). By encapsulating the MoTe2 with graphene protection layers, we create an in situ reaction cell compatible with atomic resolution imaging. We find that the Td-to-2H phase transition initiates at phase boundaries at low temperatures (200-225 degree C) and propagates anisotropically along the b-axis in a layer-by-layer fashion. We also demonstrate a fully reversible 2H-Td-2H phase transition cycle, which generates a coherent 2H lattice containing inversion domain boundaries. Our results provide insights on fabricating 2D hetero-phase devices with atomically sharp and coherent interfaces.

cond-mat.mtrl-sci↗

arXiv2022

Angstrom-Scale Imaging of Magnetization in Antiferromagnetic Fe$_2$As via 4D-STEM

We demonstrate a combination of computational tools and experimental 4D-STEM methods to image the local magnetic moment in antiferromagnetic Fe$_2$As with 6 angstrom spatial resolution. Our techniques utilize magnetic diffraction peaks, common in antiferromagnetic materials, to create imaging modes that directly visualize the magnetic lattice. Using this approach, we show that center-of-mass analysis can determine the local magnetization component in the plane perpendicular to the path of the electron beam. Moreover, we develop Magnstem, a quantum mechanical electron scattering simulation code, to model electron scattering of an angstrom-scale probe from magnetic materials. Using these tools, we identify optimal experimental conditions for separating weak magnetic signals from the much stronger interactions of an angstrom-scale probe with electrostatic potentials. Our techniques should be useful for characterizing the local magnetic order in systems such in thin films, interfaces, and domain boundaries of antiferromagnetic materials, which are difficult to probe with existing methods.

cond-mat.mtrl-sci↗

arXiv2022

High-resolution diffraction reveals magnetoelastic coupling and coherent phase separation in tetragonal CuMnAs

Tetragonal CuMnAs was the first antiferromagnet where reorientation of the Néel vector was reported to occur by an inverse spin galvanic effect. A complicating factor in the formation of phase-pure tetragonal CuMnAs is the formation of an orthorhombic phase with nearly the same stoichiometry. Pure-phase tetragonal CuMnAs has been reported to require an excess of Cu to maintain a single phase in traditional solid state synthesis reactions. Here we show that subtle differences in diffraction patterns signal pervasive inhomogeneity and phase separation, even in Cu-rich Cu$_{1.18}$Mn$_{0.82}$As. From calorimetry and magnetometry measurements, we identify two transitions corresponding to the Néel temperature (T$_N$) and an antiferromagnet to weak ferromagnet transition in Cu$_{1.18}$Mn$_{0.82}$As and CuMn$_{0.964}$As$_{1.036}$. These transitions have clear crystallographic signatures, directly observable in the lattice parameters upon in-situ heating and cooling. The immiscibility and phase separation could arise from a spinoidal decomposition that occurs at high temperatures, and the presence of a ferromagnetic transition near room temperature warrants further investigation of its effect on the electrical switching behavior.

cond-mat.mtrl-sci↗

arXiv2021

Nearly hyperuniform, nonhyperuniform, and antihyperuniform density fluctuations in two-dimensional transition metal dichalcogenides with defects

Hyperuniform many-body systems in $d$-dimensional Euclidean space are characterized by completely suppressed (normalized) infinite-wavelength density fluctuations, and appear to be endowed with novel exotic physical properties. In this work, we analyze the effects of localized defects on the density fluctuations across length scales and on the hyperuniformity property of experimental samples of two-dimensional transition metal dichalcogenides. In particular, we extract atomic coordinates from time series annular dark field-scanning transmission electron microscopy imaging data of 2D tungsten chalcogenides with the 2H structure showing continuous development and evolution of electron-beam induced defects, and construct the corresponding chemical-bonding informed coordination networks between the atoms. We then compute a variety of pair statistics and bond-orientational statistics to characterize the samples. At low defect concentrations, the corresponding materials are nearly hyperuniform. As more defects are introduced, the (approximate) hyperuniformity of the materials is gradually destroyed, and the system becomes non-hyperuniform even when the material still contains a significant amount of crystalline regions. At high defect concentrations, the structures become antihyperuniform with diverging (normalized) large-scale density fluctuations. Overall, the defected materials possess varying degrees of orientation order, and there is apparently no intermediate hexatic phase emerging. We also construct a minimalist structural model and demonstrate that the experimental samples can be essentially viewed as perturbed honeycomb crystals with small correlated displacements and double chalcogen vacancies.

cond-mat.soft↗

arXiv2020

Deep Learning Enabled Strain Mapping of Single-Atom Defects in 2D Transition Metal Dichalcogenides with Sub-picometer Precision

2D materials offer an ideal platform to study the strain fields induced by individual atomic defects, yet challenges associated with radiation damage have so-far limited electron microscopy methods to probe these atomic-scale strain fields. Here, we demonstrate an approach to probe single-atom defects with sub-picometer precision in a monolayer 2D transition metal dichalcogenide, WSe$_{2-2x}$Te$_{2x}$. We utilize deep learning to mine large datasets of aberration-corrected scanning transmission electron microscopy images to locate and classify point defects. By combining hundreds of images of nominally identical defects, we generate high signal-to-noise class-averages which allow us to measure 2D atomic coordinates with up to 0.3 pm precision. Our methods reveal that Se vacancies introduce complex, oscillating strain fields in the WSe$_{2-2x}$Te$_{2x}$ lattice which cannot be explained by continuum elastic theory. These results indicate the potential impact of computer vision for the development of high-precision electron microscopy methods for beam-sensitive materials.

cond-mat.mtrl-sci↗

arXiv2018

Strain Modulation of Graphene by Nanoscale Substrate Curvatures: A Molecular View

Spatially nonuniform strain is important for engineering the pseudomagnetic field and band structure of graphene. Despite the wide interest in strain engineering, there is still a lack of control on device-compatible strain patterns due to the limited understanding of the structure-strain relationship. Here, we study the effect of substrate corrugation and curvature on the strain profiles of graphene via combined experimental and theoretical studies of a model system: graphene on closely packed SiO2 nanospheres with different diameters (20-200 nm). Experimentally, via quantitative Raman analysis, we observe partial adhesion and wrinkle features and find that smaller nanospheres induce larger tensile strain in graphene, theoretically, molecular dynamics simulations confirm the same microscopic structure and size dependence of strain and reveal that a larger strain is caused by a stronger, inhomogeneous interaction force between smaller nanospheres and graphene. This molecular-level understanding of the strain mechanism is important for strain engineering of graphene and other two-dimensional materials.

cond-mat.mes-hall↗