arXiv subjects

Michelle A. Smeaton

Publications and source records attributed to Michelle A. Smeaton.

7 recordsLinked to original sources

arXiv2026

Face-to-face anneal temperature controls lattice parameter in Ta(C,N) virtual substrates for AlGaN power electronics

Tantalum carbide (TaC) thin film ''virtual'' substrates are a highly desirable material for $\text{Al}_{0.5}\text{Ga}_{0.5}\text{N}$ vertical power electronics devices due to lattice matching, thermal expansion matching, and metallic conductivity. However, the material has not been demonstrated to support $\text{Al}_{x}\text{Ga}_{1-x}\text{N}$ layers of variable composition $x$, limiting the range of device applications. We present a method to achieve tunable rock salt $\text{Ta}\text{C}_{x}\text{N}_{1-x}$ virtual substrates via a face-to-face annealing of TaC thin films in an $\text{N}_2$ atmosphere. The results suggest that annealing temperatures below $1600\,^{\circ}\text{C}$ promote partial uptake of nitrogen onto carbon and anion vacancy sites to form rock salt $\text{Ta(C,N)}$ with intermediate anion compositions. At temperatures $\ge 1600\,^{\circ}\text{C}$, nitrogen primarily occupies the anion sublattice and the crystalline quality and surface morphology simultaneously degrade coincident with the formation of secondary phases. This study demonstrates the growth and processing parameters necessary to make tunable lattice constant virtual substrates for $\text{Al}_{x}\text{Ga}_{1-x}\text{N}$ from $x = 0.5\text{-}1$, enabling vertically conducting power electronic devices with reduced defect density at high Al-content.

cond-mat.mtrl-sci↗

arXiv2026

Revealing epitaxial relationships at Ga$_2$O$_3$ interfaces with p-type oxides

p-type oxide contact layers such as Cr$_2$O$_3$ and NiO are attracting increasing interest in pn-heterojunctions with n-type monoclinic $β$-Ga$_2$O$_3$ for high-power electronic devices and other extreme environment applications. However, scientific understanding of their epitaxial relationships remains incomplete. In this work we investigate the epitaxial relation of Cr$_2$O$_3$ and NiO layers to (001) and ($\bar{2}$01) out-of-plane oriented Ga$_2$O$_3$ substrates. Surprisingly, we find that, for the most commercially relevant (001)-orientation of the Ga$_2$O$_3$ substrate, the epitaxial relationships are Cr$_2$O$_3$ (0001) and NiO (111) $\parallel$ Ga$_2$O$_3$ (101), both at the non-intuitive $χ$ = 22.5 $^\circ$ angle with respect to the substrate normal. We explain this unusual discovery by the interfacial atomistic bonding dominated by oxygen sublattice equivalence of these Cr$_2$O$_3$ and NiO polar surface orientations to the tilted Ga$_2$O$_3$ (101), rather than Ga$_2$O$_3$ (001) substrate surface planes. Furthermore, we assign the in-plane orientation for Cr$_2$O$_3$ on ($\bar{2}$01)-oriented Ga$_2$O$_3$ as: Cr$_2$O$_3$ $[12\bar{3}0]$ $\parallel$ Ga$_2$O$_3$ $[010]$ with two in-plane rotational domains. Interface modeling confirms the in-plane orientation for Cr$_2$O$_3$/$(\bar{2}01)$ Ga$_2$O$_3$ and shows that strained O-terminated Ga$_2$O$_3$ $(\bar{2}01)$ surfaces have the lowest interfacial energy with Cr$_2$O$_3$ (0001). Beyond establishing the specific epitaxial relationships for Cr$_2$O$_3$ and NiO on Ga$_2$O$_3$, this work provides a systematic methodology for the unambiguous structural characterization of heterointerfaces involving materials with markedly different crystal symmetries.

cond-mat.mtrl-sci↗

arXiv2026

Revealing the Atomic Structure of NiO/Ga$_{2}$O$_{3}$ Interfaces

NiO/Ga$_{2}$O$_{3}$ heterojunctions have garnered significant attention for use in power electronics due to the ultrawide bandgap and wafer-scale availability of Ga$_{2}$O$_{3}$ and the controllable p-type doping of NiO. However, the structure of NiO/Ga$_{2}$O$_{3}$ interfaces remains underexplored, largely due to the complexity of the junction between their dissimilar cubic and monoclinic crystal structures. Here we investigate the atomistic structure of the NiO/Ga$_{2}$O$_{3}$ interface for (100), (-201), and (001) oriented Ga$_{2}$O$_{3}$ substrates using aberration-corrected scanning transmission electron microscopy (STEM) in combination with interface modeling and image simulations. We evaluate the abruptness and consistency of the interfaces and compare them to calculated interface models, proposing precise atomic structures and assessing potential structural variation arising from complexity of the monoclinic Ga$_{2}$O$_{3}$ crystal structure. Our interface analysis supports increased focus on (100) oriented Ga$_{2}$O$_{3}$ as a candidate for fabricating high quality, low defect density NiO/Ga$_{2}$O$_{3}$ heterojunction devices. Importantly, we consider the effects of specimen thickness and 3D-to-2D projection during the STEM imaging process to differentiate such effects from real crystal variations. This work provides insight into the effect of substrate orientation on NiO film and interface quality, creating a pathway to improving heterojunction properties. It further highlights important considerations for interpretation of stability and interlayer phase formation in these interfaces, which is crucial for their integration into reliable and robust power electronic devices.

cond-mat.mtrl-sci↗

arXiv2026

Born-Qualified: An Autonomous Framework for Deploying Advanced Energy and Electronic Materials

Autonomous science is transforming how we discover materials and chemical systems for advanced energy technologies. However, many initially promising systems never reach deployment. This "valley of death" stems from optimization that prioritizes laboratory metrics over industrial viability. We propose a new strategy: "born-qualified" autonomous development, which embeds manufacturability, cost, and durability constraints from the outset. This approach is enabled by four pillars, including the development of multi-objective metrics, causal models, a modular infrastructure, and embedding manufacturing in the discovery loop. Realizing this vision will require sustained, community-wide commitment, but the potential return on that investment is commensurate with the scale of the challenge.

cond-mat.mtrl-sci↗

arXiv2025

Revealing the Hidden Third Dimension of Point Defects in Two-Dimensional MXenes

Point defects govern many important functional properties of two-dimensional (2D) materials. However, resolving the three-dimensional (3D) arrangement of these defects in multi-layer 2D materials remains a fundamental challenge, hindering rational defect engineering. Here, we overcome this limitation using an artificial intelligence-guided electron microscopy workflow to map the 3D topology and clustering of atomic vacancies in Ti$_3$C$_2$T$_X$ MXene. Our approach reconstructs the 3D coordinates of vacancies across hundreds of thousands of lattice sites, generating robust statistical insight into their distribution that can be correlated with specific synthesis pathways. This large-scale data enables us to classify a hierarchy of defect structures--from isolated vacancies to nanopores--revealing their preferred formation and interaction mechanisms, as corroborated by molecular dynamics simulations. This work provides a generalizable framework for understanding and ultimately controlling point defects across large volumes, paving the way for the rational design of defect-engineered functional 2D materials.

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

Mind the Gap: Bridging the Divide Between AI Aspirations and the Reality of Autonomous Characterization

What does materials science look like in the "Age of Artificial Intelligence?" Each materials domain-synthesis, characterization, and modeling-has a different answer to this question, motivated by unique challenges and constraints. This work focuses on the tremendous potential of autonomous characterization within electron microscopy. We present our recent advancements in developing domain-aware, multimodal models for microscopy analysis capable of describing complex atomic systems. We then address the critical gap between the theoretical promise of autonomous microscopy and its current practical limitations, showcasing recent successes while highlighting the necessary developments to achieve robust, real-world autonomy.

cond-mat.mtrl-sci↗