arXiv subjects

Celesta S. Chang

Publications and source records attributed to Celesta S. Chang.

15 recordsLinked to original sources

arXiv2026

Optimization-Based Thickness Estimation and Depth-Resolved FIB-Induced Damage Characterization via Multislice Electron Ptychography

Quantitative electron microscopy requires accurate knowledge of specimen thickness because dynamical scattering strongly affects image contrast and diffraction intensities. In multislice electron ptychography (MEP), specimen thickness is a required input parameter to its forward model, yet the local thickness of a transmission electron microscope (TEM) lamella is often precisely what is unknown. Moreover, thickness is coupled to probe defocus and the number of slices, making its determination from the reconstruction itself nontrivial. Here, we assess whether joint Bayesian optimization of these parameters can provide a physically meaningful estimate of local thickness from four-dimensional scanning transmission electron microscopy (4D-STEM) data. Applied to a wedge-shaped silicon lamella, the optimization reproduced similar local thickness variation measured by electron energy loss spectroscopy (EELS), with a systematic offset of 10-17% relative to the EELS estimates. Using the optimized reconstruction parameters, depth-resolved MEP further separated the crystalline silicon interior from focused ion beam (FIB)-induced amorphous surface layers within the same reconstructed volume. Regions milled at final voltages of 2, 5, 8, and 30 kV yielded amorphous-layer thicknesses of 3.2, 5.0, 7.0, and 26.4 nm, respectively, increasing monotonically with milling voltage and agreeing reasonably with previous cross-sectional measurements. These results show that applying MEP coupled with Bayesian optimization on a single 4D-STEM dataset can provide both local thickness estimates and depth-resolved characterization of FIB-induced damage, offering a route toward more self-consistent, thickness-aware quantitative 4D-STEM analysis.

cond-mat.mtrl-sci↗

arXiv2026

Three-Dimensional Imaging of High-Density Dislocation Networks and Their Interactions using Multislice Electron Ptychography

Development of novel devices often involve combining functional materials and substrates, each chosen for particular physical properties such as low-loss or thermal conductivity. This, however, can introduce a large lattice mismatch and high density of structural defects that may limit device performance and reliability by trapping charge or creating leakage pathways. Such is the case for integrating superconducting TiN with a low-loss sapphire substrate. Here we resolve and image the resulting misfit, screw, and threading dislocations in epitaxial TiN on sapphire using the depth-sectioning capabilities of multislice electron ptychography. We find misfit dislocations spaced ~1.6 nm apart and track out-of-plane crossings of misfit dislocations as well as their transitions to threading dislocations, details which are obscured in conventional defect-imaging methods. The ability to correlate specific dislocation types and their interactions in extremely small volumes and at high densities is valuable for understanding structure-property relations even in modern, scaled devices.

cond-mat.mtrl-sci↗

arXiv2026

High-Q superconducting microwave resonators using MBE titanium nitride

Using molecular beam epitaxy, we have realized thin films of titanium nitride (TiN) on c-plane sapphire that exhibit the lowest observed full-width at half maximum X-ray rocking curve width of 18 arcsec. Though the (111) oriented TiN exhibits an abrupt and crystalline interface with sapphire, for the first time we observe sub-surface defects in the sapphire substrate, which nucleate structural defects in the epitaxial TiN layer. Using quarter-wavelength coplanar waveguide (CPW) resonators in a 3 \textmu m/6 \textmu m/3 \textmu m gap/strip/gap lines in a hanger geometry, we find the internal quality factor of the TiN resonators to be $>10^{6}$ in the single-photon $\langle n \rangle \sim 1$ limit at 5.8 GHz and 10 mK, rising to $>20 \times 10^{6}$ at $\langle n \rangle \sim 10^{6}$. The results are of high interest for applications of superconducting TiN in several areas, and provide a path towards epitaxial Josephson junctions with crystalline barriers in the future for high coherence qubits.

cond-mat.supr-con↗

arXiv2026

Strain-tuned orbital-dependent electronic correlations in FeTe thin films

Iron chalcogenides exhibit rich phenomena which are governed by orbital-dependent electronic interactions and strong electronic correlation. In particular, many studies have explored orbital selectivity in FeTe through Se doping. Here, applying tensile strain to thin films allows us to precisely control the system without other impurities that may arise from chemical doping to investigate the emergent behaviors in FeTe. Using angle-resolved photoemission spectroscopy, we observe a spectral weight transfer between $d_{\rm xy}$ and $d_{\rm z^{2}}$ orbitals, evidence of an orbital-selective Mott phase (OSMP). Beyond OSMP, we reveal hitherto unobserved strain-induced effects, distinct from chemical doping. The evolution of $d_{\rm xz}$ orbital demonstrates how electron hopping mechanism plays an important role in defining the electronic properties of the system. Our findings highlight a direct correlation between epitaxial strain and the evolution of electronic structures in FeTe.

cond-mat.str-el↗

arXiv2023

Pulsed-mode metalorganic vapor-phase epitaxy of GaN on graphene-coated c-sapphire for freestanding GaN thin films

We report the growth of high-quality GaN epitaxial thin films on graphene-coated c-sapphire substrates using pulsed-mode metalorganic vapor-phase epitaxy, together with the fabrication of freestanding GaN films by simple mechanical exfoliation for transferable light-emitting diodes (LEDs). High-quality GaN films grown on the graphene-coated sapphire substrates were easily lifted off using thermal release tape and transferred onto foreign substrates. Furthermore, we revealed that the pulsed operation of ammonia flow during GaN growth was a critical factor for the fabrication of high-quality freestanding GaN films. These films, exhibiting excellent single crystallinity, were utilized to fabricate transferable GaN LEDs by heteroepitaxially growing InxGa1-xN/GaN multiple quantum wells and a p-GaN layer on the GaN films, showing their potential application in advanced optoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2022

Multiplication of freestanding semiconductor membranes from a single wafer by advanced remote epitaxy

Freestanding single-crystalline membranes are an important building block for functional electronics. Especially, compounds semiconductor membranes such as III-N and III-V offer great opportunities for optoelectronics, high-power electronics, and high-speed computing. Despite huge efforts to produce such membranes by detaching epitaxial layers from donor wafers, however, it is still challenging to harvest epitaxial layers using practical processes. Here, we demonstrate a method to grow and harvest multiple epitaxial membranes with extremely high throughput at the wafer scale. For this, 2D materials are directly formed on III-N and III-V substrates in epitaxy systems, which enables an advanced remote epitaxy scheme comprised of multiple alternating layers of 2D materials and epitaxial layers that can be formed by a single epitaxy run. Each epilayer in the multi-stack structure is then harvested by layer-by-layer peeling, producing multiple freestanding membranes with unprecedented throughput from a single wafer. Because 2D materials allow peeling at the interface without damaging the epilayer or the substrate, wafers can be reused for subsequent membrane production. Therefore, this work represents a meaningful step toward high-throughput and low-cost production of single-crystal membranes that can be heterointegrated.

physics.app-ph↗

arXiv2022

Disentangling magnetic and grain contrast in polycrystalline FeGe thin films using four-dimensional Lorentz scanning transmission electron microscopy

The study of nanoscale chiral magnetic order in polycrystalline materials with a strong Dzyaloshinkii-Moriya interaction (DMI) is interesting for the observation of magnetic phenomena at grain boundaries and interfaces. One such material is sputter-deposited B20 FeGe on Si, which has been actively investigated as the basis for low-power, high-density magnetic memory technology in a scalable material platform. Although conventional Lorentz electron microscopy provides the requisite spatial resolution to probe chiral magnetic textures in single-crystal FeGe, probing the magnetism of sputtered B20 FeGe is more challenging because the sub-micron crystal grains add confounding contrast. We address the challenge of disentangling magnetic and grain contrast by applying 4-dimensional Lorentz scanning transmission electron microscopy using an electron microscope pixel array detector. Supported by analytical and numerical models, we find that the most important parameter for imaging magnetic materials with polycrystalline grains is the ability for the detector to sustain large electron doses, where having a high-dynamic range detector becomes extremely important. Despite the small grain size in sputtered B20 FeGe on Si, using this approach we are still able to observe helicity switching of skyrmions and magnetic helices across two adjacent grains as they thread through neighboring grains. We reproduce this effect using micromagnetic simulations by assuming that the grains have distinct orientation and magnetic chirality and find that magnetic helicity couples to crystal chirality. Our methodology for imaging magnetic textures is applicable to other thin-film magnets used for spintronics and memory applications, where an understanding of how magnetic order is accommodated in polycrystalline materials is important.

cond-mat.mtrl-sci↗

arXiv2021

Momentum-resolved electronic band structure and offsets in an epitaxial NbN/GaN superconductor/semiconductor heterojunction

The electronic structure of heterointerfaces play a pivotal role in their device functionality. Recently, highly crystalline ultrathin films of superconducting NbN have been integrated by molecular beam epitaxy with the semiconducting GaN. We use soft X-ray angle-resolved photoelectron spectroscopy to directly measure the momentum-resolved electronic band structures for both NbN and GaN constituents of this Schottky heterointerface, and determine their momentum-dependent interfacial band offset as well as the band-bending profile into GaN. We find, in particular, that the Fermi states in NbN are aligned against the band gap in GaN, which excludes any significant electronic cross-talk of the superconducting states in NbN through the interface to GaN. We support the experimental findings with first-principles calculations for bulk NbN and GaN. The Schottky barrier height obtained from photoemission is corroborated by electronic transport and optical measurements. The momentum-resolved understanding of electronic properties elucidated by the combined materials advances and experimental methods in our work opens up new possibilities in systems where interfacial states play a defining role.

cond-mat.mtrl-sci↗

arXiv2020

Transferring Orbital Angular Momentum to an Electron Beam Reveals Toroidal and Chiral Order

Orbital angular momentum and torque transfer play central roles in a wide range of magnetic textures and devices including skyrmions and spin-torque electronics(1-4). Analogous topological structures are now also being explored in ferroelectrics, including polarization vortex arrays in ferroelectric/dielectric superlattices(5). Unlike magnetic toroidal order, electric toroidal order does not couple directly to linear external fields. To develop a mechanism that can control switching in polarization vortices, we utilize a high-energy electron beam and show that transverse currents are generated by polar order in the ballistic limit. We find that the presence of an electric toroidal moment in a ferro-rotational phase transfers a measurable torque and orbital angular momentum to the electron beam. Furthermore, we find that the complex polarization patterns, observed in these heterostructures, are microscopically chiral with a non-trivial axial component of the polarization. This chirality opens the door for the coupling of ferroelectric and optical properties.

cond-mat.mtrl-sci↗

arXiv2020

$γ$-phase Inclusions as Common Defects in Alloyed $β$-(Al$_x$Ga$_{1\text{-}x}$)$_2$O$_3$ and Doped $β$-Ga$_2$O$_3$ Films

$β$-Ga$_2$O$_3$ is a promising ultra-wide bandgap semiconductor whose properties can be further enhanced by alloying with Al. Here, using atomic-resolution scanning transmission electron microscopy (STEM), we find the thermodynamically-unstable $γ$-phase is a ubiquitous defect in both $β$-(Al$_x$Ga$_{1\text{-}x}$)$_2$O$_3$ films and doped $β$-Ga$_2$O$_3$ films grown by molecular beam epitaxy. For undoped $β$-(Al$_x$Ga$_{1\text{-}x}$)$_2$O$_3$ films we observe $γ$-phase inclusions between nucleating islands of the $β$-phase at lower growth temperatures (~400-600 $^{\circ}$C). In doped $β$-Ga$_2$O$_3$, a thin layer of the $γ$-phase is observed on the surfaces of films grown with a wide range of n-type dopants and dopant concentrations. The thickness of the $γ$-phase layer was most strongly correlated with the growth temperature, peaking at about 600 $^{\circ}$C. Ga interstitials are observed in $β$-phase, especially near the interface with the $γ$-phase. By imaging the same region of the surface of a Sn-doped $β$-(Al$_x$Ga$_{1\text{-}x}$)$_2$O$_3$ after ex-situ heating up to 400 $^{\circ}$C, a $γ$-phase region is observed to grow above the initial surface, accompanied by a decrease in Ga interstitials in the $β$-phase. This suggests that the diffusion of Ga interstitials towards the surface is likely the mechanism for growth of the surface $γ$-phase, and more generally that the more-open $γ$-phase may offer diffusion pathways to be a kinetically-favored and early-forming phase in the growth of Ga$_2$O$_3$.

cond-mat.mtrl-sci↗

arXiv2020

Adsorption-Controlled Growth of Ga2O3 by Suboxide Molecular-Beam Epitaxy

This paper introduces a growth method---suboxide molecular-beam epitaxy (S-MBE)---which enables the growth of Ga2O3 and related materials at growth rates exceeding 1 micrometer per hours with excellent crystallinity in an adsorptioncontrolled regime. Using a Ga + Ga2O3 mixture with an oxygen mole fraction of x(O) = 0.4 as an MBE source, we overcome kinetic limits that had previously hampered the adsorption-controlled growth of Ga2O3 by MBE. We present growth rates up to 1.6 micrometer per hour for Ga2O3--Al2O3 heterostructures with unprecedented crystalline quality and also at unparalleled low growth temperature for this level of perfection. We combine thermodynamic knowledge of how to create molecular-beams of targeted suboxides with a kinetic model developed for the S-MBE of III-VI compounds to identify appropriate growth conditions. Using S-MBE we demonstrate the growth of phase-pure, smooth, and high-purity homoepitaxial Ga2O3 films that are thicker than 4 micrometer. With the high growth rate of S-MBE we anticipate a significant improvement to vertical Ga2O3-based devices. We describe and demonstrate how this growth method can be applied to a wide-range of oxides. S-MBE rivals leading synthesis methods currently used for the production of Ga2O3-based devices.

cond-mat.mtrl-sci↗

arXiv2020

Crystal orientation dictated epitaxy of ultrawide bandgap 5.4-8.6 eV $α$-(AlGa)$_2$O$_3$ on m-plane sapphire

Ultra-wide bandgap semiconductors are ushering in the next generation of high power electronics. The correct crystal orientation can make or break successful epitaxy of such semiconductors. Here it is discovered that single-crystalline layers of $α$-(AlGa)$_2$O$_3$ alloys spanning bandgaps of 5.4 - 8.6 eV can be grown by molecular beam epitaxy. The key step is found to be the use of m-plane sapphire crystal. The phase transition of the epitaxial layers from the $α$- to the narrower bandgap $β$-phase is catalyzed by the c-plane of the crystal. Because the c-plane is orthogonal to the growth front of the m-plane surface of the crystal, the narrower bandgap pathways are eliminated, revealing a route to much wider bandgap materials with structural purity. The resulting energy bandgaps of the epitaxial layers span a range beyond the reach of all other semiconductor families, heralding the successful epitaxial stabilization of the largest bandgap materials family to date.

physics.app-ph↗

arXiv2020

In situ modification of delafossite type PdCoO2 bulk single crystal for reversible hydrogen sorption and fast hydrogen evolution

The observation of extraordinarily high conductivity in delafossite-type PdCoO2 is of great current interest, and there is some evidence that electrons behave like a fluid when flowing in bulk crystals of PdCoO2. Thus, this material is an ideal platform for the study of the electron transfer processes in heterogeneous reactions. Here, we report the use of bulk single crystal PdCoO2 as a promising electrocatalyst for hydrogen evolution reactions (HERs). An overpotential of only 31 mV results in a current density of 10 mA cm^(-2), accompanied by high long-term stability. We have precisely determined that the crystal surface structure is modified after electrochemical activation with the formation of strained Pd nanoclusters in the surface layer. These nanoclusters exhibit reversible hydrogen sorption and desorption, creating more active sites for hydrogen access. The bulk PdCoO2 single crystal with ultra-high conductivity, which acts as a natural substrate for the Pd nanoclusters, provides a high-speed channel for electron transfer

cond-mat.mtrl-sci↗

arXiv2018

Exceptionally high, strongly temperature dependent, spin Hall conductivity of SrRuO3

Spin-orbit torques (SOT) in thin film heterostructures originate from strong spin-orbit interactions (SOI) that, in the bulk, generate a spin current as the result of extrinsic spin-dependent, skew or/and side-jump, scattering, or in the intrinsic case due to Berry curvature in the conduction band. While most SOT studies have focused on materials with heavy metal components, the oxide perovskite SrRuO3 has been predicted to have a pronounced Berry curvature. Through quantification of its spin current by the SOT exerted on an adjacent Co ferromagnetic layer, we determine that SrRuO3 has a strongly temperature (T) dependent spin Hall conductivity which becomes particularly high at low T, e.g. σ_{SH} \geqslant (\hbar/2e)3x10^{5} Ω^{-1}m^{-1} at 60 K. Below the SrRuO3 ferromagnetic transition, non-standard SOT components develop associated with the magnetic characteristics of the oxide, but these do not dominate as with spin currents from a conventional ferromagnet. Our results establish a new approach for the study of SOI in epitaxial conducting oxide heterostructures and confirm SrRuO3 as a promising candidate material for achieving new and enhanced spintronics functionalities.

cond-mat.mtrl-sci↗

arXiv2015

High Dynamic Range Pixel Array Detector for Scanning Transmission Electron Microscopy

We describe a hybrid pixel array detector (EMPAD - electron microscope pixel array detector) adapted for use in electron microscope applications, especially as a universal detector for scanning transmission electron microscopy. The 128 x 128 pixel detector consists of a 500 um thick silicon diode array bump-bonded pixel-by-pixel to an application-specific integrated circuit (ASIC). The in-pixel circuitry provides a 1,000,000:1 dynamic range within a single frame, allowing the direct electron beam to be imaged while still maintaining single electron sensitivity. A 1.1 kHz framing rate enables rapid data collection and minimizes sample drift distortions while scanning. By capturing the entire unsaturated diffraction pattern in scanning mode, one can simultaneously capture bright field, dark field, and phase contrast information, as well as being able to analyze the full scattering distribution, allowing true center of mass imaging. The scattering is recorded on an absolute scale, so that information such as local sample thickness can be directly determined. This paper describes the detector architecture, data acquisition (DAQ) system, and preliminary results from experiments with 80 to 200 keV electron beams.

physics.ins-det↗