arXiv subjects

Thomas S. Marchese

Publications and source records attributed to Thomas S. Marchese.

4 recordsLinked to original sources

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↗

arXiv2024

Guidelines for Correlative Imaging and Analysis of Reactive Lithium Metal Battery Materials

To unlock the full potential of lithium metal batteries, a deep understanding of lithium metal reactivity and its solid electrolyte interphase is essential. Correlative imaging, combining focused ion beam and electron microscopy offers a powerful approach for multi-scale characterization. However, the extreme reactivity of lithium metal and its SEI presents challenges in investigating deposition and stripping mechanisms. In this work, we systematically evaluated the storage stability of lithium metal in glovebox before and after electrochemical deposition. We then assessed different FIB ion sources for their impact on lithium metal lamella preparation for transmission electron microscopy. Furthermore, we examined cryogenic-TEM transfer methods, optimizing for minimal contamination during sample handling. Contrary to prior assumptions, we demonstrate that high resolution imaging of pure lithium metal at room temperature is achievable using inert gas transfer with an electron dose rate exceeding 1000 e/A2/s, without significant detectable damage. In contrast, SEI components, such as Li2CO3 and LiF display much greater sensitivity to electron beams, requiring cryogenic conditions and precise dose control for nano/atomic scale imaging. We quantified electron dose limits for these SEI components to track their structural evolution under irradiation. Based on these findings, we propose a robust protocol for lithium metal sample handling - from storage to atomic-level characterization - minimizing damage and contamination. This work paves the way for more accurate and reproducible studies, accelerating the development of next-generation lithium metal batteries by ensuing the preservation of native material properties during analysis.

cond-mat.mtrl-sci↗

arXiv2024

Preservation of Topological Surface States in Millimeter-Scale Transferred Membranes

Ultrathin topological insulator membranes are building blocks of exotic quantum matter. However, traditional epitaxy of these materials does not facilitate stacking in arbitrary orders, while mechanical exfoliation from bulk crystals is also challenging due to the non-negligible interlayer coupling therein. Here we liberate millimeter-scale films of topological insulator Bi$_2$Se$_3$, grown by molecular beam epitaxy, down to 3 quintuple layers. We characterize the preservation of the topological surface states and quantum well states in transferred Bi$_{2}$Se$_{3}$ films using angle-resolved photoemission spectroscopy. Leveraging the photon-energy-dependent surface sensitivity, the photoemission spectra taken with $6$ eV and $21.2$ eV photons reveal a transfer-induced migration of the topological surface states from the top to the inner layers. By establishing clear electronic structures of the transferred films and unveiling the wavefunction relocation of the topological surface states, our work paves the physics foundation crucial for the future fabrication of artificially stacked topological materials with single-layer precision.

cond-mat.mtrl-sci↗

arXiv2023

Elucidating Dynamic Conductive State Changes in Amorphous Lithium Lanthanum Titanate for Resistive Switching Devices

Exploration of novel resistive switching materials attracts attention to replace conventional Si-based transistors and to achieve neuromorphic computing that can surpass the limit of the current Von-Neumann computing for the time of Internet of Things (IoT). Materials priorly used to serve in batteries have demonstrated metal-insulator transitions upon an electrical biasing due to resulting compositional change. This property is desirable for future resistive switching devices. Amorphous lithium lanthanum titanate (a-LLTO) was originally developed as a solid-state electrolyte with relatively high lithium ionic conductivity and low electronic conductivity among oxide-type solid electrolytes. However, it has been suggested that electric conductivity of a-LLTO changes depending on oxygen content. In this work, the investigation of switching behavior of a-LLTO was conducted by employing a range of voltage sweep techniques, ultimately establishing a stable and optimal operating condition within the voltage window of -3.5 V to 3.5 V. This voltage range effectively balances the desirable trait of a substantial resistance change by three orders of magnitude with the imperative avoidance of LLTO decomposition. This switching behavior is also confirmed at nanodevice of Ni/LLTO/Ni through in-situ biasing inside focused-ion beam/scanning electron microscope (FIB-SEM). Experiment and computation with different LLTO composition shows that LLTO has two distinct conductivity states due to Ti reduction. The distribution of these two states is discussed using simplified binary model, implying the conductive filament growth during low resistance state. Consequently, our study deepens understanding of LLTO electronic properties and encourages the interdisciplinary application of battery materials for resistive switching devices.

physics.app-ph↗