arXiv subjects

Harish Kumarasubramanian

Publications and source records attributed to Harish Kumarasubramanian.

9 recordsLinked to original sources

arXiv2026

Revealing buried ferroelectric topologies by depth-resolved electron diffraction imaging

Nanoscale topological polar textures promise new functionalities for ferroelectric memories and logic, yet their three-dimensional structure and mesoscale organization remain experimentally inaccessible. Here we introduce depth-resolved electron diffraction imaging (DREDI), a fast, non-destructive, method that maps polarization with <50 nm lateral and <10 nm depth sensitivity within fraction of a second. Its high acquisition speed enables the first continuous polarization mapping across six orders of magnitude in length scale, from nanometers to millimeters. Using epitaxial BiFeO3 films, DREDI reveals a hidden depth evolution of polar textures: surface 71-degree stripes evolve into subsurface flux-closure vortices that bifurcate into three-fold vertices near the bottom interface. Cross-sectional multi-slice electron ptychography and phase-field modeling confirm these buried configurations and attribute them to strain heterogeneity and ferroelastic twinning in the SrRuO3 electrode. Large-area analysis further shows that vertex-like frustration forms a mesoscale percolating network above a critical length scale of 4 um. DREDI enables real-time, volumetric studies of buried topological textures in ferroic nanomaterials.

cond-mat.mtrl-sci↗

arXiv2025

Chemical state detection and charge transfer in complex oxide heterostructures via in situ Auger Electron Spectroscopy

Understanding and controlling the chemical states both in the bulk and at the interfaces of complex oxide thin films is essential for engineering a wide range of electronic, optical, and magnetic functionalities, which arise through emergent phenomena such as two-dimensional electron gases, interfacial magnetism, and associated phase transitions. Here, we demonstrate the use of in situ Auger Electron Spectroscopy (AES) as a powerful tool for probing oxidation states and dynamic chemical processes during the growth of complex oxide heterostructures. By leveraging the chemical sensitivity of AES to subtle changes in valence electron populations, we show that this technique can distinguish distinct oxidation states in multivalent perovskite manganate and vanadate systems with high fidelity during deposition. Furthermore, we show evidence for dynamic chemical phenomena, specifically charge transfer processes at the polar-nonpolar LaMnO3/SrTiO3 interface. Our results establish in situ AES as a powerful diagnostic tool for monitoring and controlling interfacial chemistry during thin film growth, offering a pathway toward the atomic-scale engineering of chemical states in functional oxide heterostructures.

cond-mat.mtrl-sci↗

arXiv2025

Textured growth and electrical characterization of Zinc Sulfide on back-end-of-the-line (BEOL) compatible substrates

Scaling of transistors has enabled continuous improvements in logic device performance, especially through materials engineering. However, surpassing horizontal limitations in chip manufacturing requires a vertical, third dimension. Three-dimensional integration of high-performance logic demands solving the challenge of low-temperature (less than 450°C) synthesis of high-mobility n-type and p-type semiconductor thin films for back-end-of-line (BEOL) compatible transistors. Metal oxides, particularly indium oxides alloyed with gallium and tungsten, are promising n-type channel materials, but suitable p-type materials for BEOL remain scarce. Zinc sulfide (ZnS), a wide band-gap semiconductor, shows room-temperature p-type conductivity when doped with copper and crystallizes below 400°C. Here, we report growth of crystalline ZnS thin films by pulsed laser deposition on amorphous and polycrystalline surfaces including silicon nitride, thermal silicon dioxide, yttrium oxide, hafnium dioxide, sapphire, platinum, and titanium nitride. X-ray diffraction reveals out-of-plane texturing across all surfaces, while grazing incidence wide-angle X-ray scattering probes in-plane crystalline quality. Surface and interface properties are assessed using X-ray reflectivity and atomic force microscopy. Electrical characterization via J-V measurements (ZnS on Pt) and metal-oxide-semiconductor capacitor (ZnS on silicon dioxide) measurements show low leakage current ($10^{-5} A/cm^2$ at 0.40 MV/cm) and bilayer capacitor behavior, suggesting ZnS is highly intrinsic with minimal electrically active defects. Further work on doping ZnS with copper or other p-type elements is needed to realize ZnS as a dopable wide band-gap semiconductor for BEOL integration. This work demonstrates a novel thin-film growth method for sulfide semiconductors under BEOL-compatible conditions.

cond-mat.mtrl-sci↗

arXiv2024

A strategy for fabricating micro-scale freestanding single-crystalline complex oxide device arrays

We present a general fabrication strategy for freestanding single-crystalline complex oxide device arrays via wet chemical etching-based microfabrication processes and epitaxial lift-off. Here, we used 0.5Ba(Zr$_{0.2}$Ti$_{0.8}$)O$_3$-0.5Ba(Zr$_{0.7}$Ti$_{0.3}$)O$_3$ (BCZT) as a model relaxor ferroelectric oxide system and La$_{0.7}$Sr$_{0.3}$MnO$_3$ as the sacrificial layer for demonstration. Arrays of SrRuO$_3$ (SRO) / BCZT / SRO ferroelectric capacitor mesas were first defined and isolated on the growth wafer, and then they were released using epitaxial lift-off with lithography-defined surrounding etching holes, after which the freestanding device arrays were integrated onto a glass substrate. Our proposed strategy sheds light on preparing various freestanding single-crystalline oxide devices and paves the way for their heterogeneous integration onto arbitrary substates.

cond-mat.mtrl-sci↗

arXiv2024

Kinetic control of ferroelectricity in ultrathin epitaxial Barium Titanate capacitors

Ferroelectricity is characterized by the presence of spontaneous and switchable macroscopic polarization. Scaling limits of ferroelectricity have been of both fundamental and technological importance, but the probes of ferroelectricity have often been indirect due to confounding factors such as leakage in the direct electrical measurements. Recent interest in low-voltage switching electronic devices squarely puts the focus on ultrathin limits of ferroelectricity in an electronic device form, specifically on the robustness of ferroelectric characteristics such as retention and endurance for practical applications. Here, we illustrate how manipulating the kinetic energy of the plasma plume during pulsed laser deposition can yield ultrathin ferroelectric capacitor heterostructures with high bulk and interface quality, significantly low leakage currents and a broad "growth window". These heterostructures venture into previously unexplored aspects of ferroelectric properties, showcasing ultralow switching voltages ($<$0.3 V), long retention times ($>$10$^{4}$s), and high endurance ($>$10$^{11}$cycles) in 20 nm films of the prototypical perovskite ferroelectric, BaTiO$_{3}$. Our work demonstrates that materials engineering can push the envelope of performance for ferroelectric materials and devices at the ultrathin limit and opens a direct, reliable and scalable pathway to practical applications of ferroelectrics in ultralow voltage switches for logic and memory technologies.

physics.app-ph↗

arXiv2024

Growth of VO2-ZnS Thin Film Cavity for Adaptive Thermal Emission

Low-weight, passive, thermal-adaptive radiation technologies are needed to maintain an operable temperature for spacecraft while they experience various energy fluxes. In this study, we used a thin-film coating with the Fabry-Perot (FP) effect to enhance emissivity contrast (Δε) between VO2 phase-change states. This coating utilizes a novel hybrid material architecture that combines VO2 with a mid- and long-wave infrared transparent chalcogenide, zinc sulfide (ZnS), as a cavity spacer layer. We simulated the design parameter space to obtain a theoretical maximum Δε of 0.63 and grew prototype devices. Using X-ray diffraction, Raman spectroscopy, and Fourier Transform Infrared (FTIR) Spectroscopy, we determined that an intermediate buffer layer of TiO2 is necessary to execute the crystalline growth of monoclinic VO2 on ZnS. Through temperature-dependent FTIR spectroscopy measurements, our fabricated devices demonstrated FP-cavity enhanced adaptive thermal emittance.

physics.optics↗

arXiv2024

Epitaxial rare-earth doped complex oxide thin films for infrared applications

Rare earth dopants are one of the most extensively studied optical emission centers for a broad range of applications such as laser optoelectronics, sensing, lighting, and quantum information technologies due to their narrow optical linewidth and exceptional coherence properties. Epitaxial doped oxide thin films can serve as a promising and controlled host to investigate rare-earth dopants suitable for scalable quantum memories, on-chip lasers and amplifiers. Here, we report high-quality epitaxial thin films of Tm-doped CaZrO$_3$ grown by pulsed laser deposition for infrared optoelectronic and quantum memory applications. We perform extensive structural and chemical characterization to probe the crystallinity of the films and the doping behavior. Low temperature photoluminescence measurements show sharp radiative transitions in the short-wave infrared range of 1.75 - 2 μm.

physics.optics↗

arXiv2021

In situ Monitoring of Composition and Sensitivity to Growth Parameters of Pulsed Laser Deposition

Complex oxide perovskites have been widely studied for their diverse functional properties. When dimensionally reduced to epitaxial thin films and heterostructures these properties are frequently tunable, and the symmetry-breaking inherent to thin film structures can result in the emergence of new, novel, phenomena and properties. However, the ability to control and harness these structures relies on an atomic-level understanding and control of the growth process, made challenging by the lack of suitable in situ compositional characterization tools. In this work, the compositional-dependence of SrTiO3 on pulsed laser deposition growth parameters is investigated with in situ Auger electron spectroscopy and ex situ thin film x-ray diffraction, and verified with a simple escape depth model. We show that this is a suitable technique for monitoring subtle compositional shifts occurring during the deposition process, with broad implications for the continued development of thin film synthesis techniques.

cond-mat.mtrl-sci↗

arXiv2021

Direct Observation and Control of Surface Termination in Perovskite Oxide Heterostructures

The interfacial behavior of quantum materials leads to emergent phenomena such as two dimensional electron gases, quantum phase transitions, and metastable functional phases. Probes for in situ and real time surface sensitive characterization are critical for active monitoring and control of epitaxial synthesis, and hence the atomic-scale engineering of heterostructures and superlattices. Termination switching, especially as an interfacial process in ternary complex oxides, has been studied using a variety of probes, often ex situ; however, direct observation of this phenomena is lacking. To address this need, we establish in situ and real time reflection high energy electron diffraction and Auger electron spectroscopy for pulsed laser deposition, which provide structural and compositional information of the surface during film deposition. Using this unique capability, we show, for the first time, the direct observation and control of surface termination in complex oxide heterostructures of SrTiO3 and SrRuO3. Density-functional-theory calculations capture the energetics and stability of the observed structures and elucidate their electronic behavior. This demonstration opens up a novel approach to monitor and control the composition of materials at the atomic scale to enable next-generation heterostructures for control over emergent phenomena, as well as electronics, photonics, and energy applications.

cond-mat.mtrl-sci↗