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Sharma, Yogesh

Publications and source records attributed to Sharma, Yogesh.

13 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Heterogeneous Integration of Freestanding Bilayer Oxide Membrane for Multiferroicity

Transition metal oxides exhibit a plethora of electrical and magnetic properties described by their order parameters. In particular, ferroic orderings offer access to a rich spectrum of fundamental physics phenomena, in addition to a range of technological applications. The heterogeneous integration of ferroelectric and ferromagnetic materials is a fruitful way to design multiferroic oxides. The realization of freestanding heterogeneous membranes of multiferroic oxides is highly desirable. In this study, epitaxial BaTiO 3 /La 0.7 Sr 0.3 MnO 3 freestanding bilayer membranes are fabricated using pulsed laser epitaxy. The membrane displays ferroelectricity and ferromagnetism above room temperature accompanying the finite magnetoelectric coupling constant. Further, this study reveals that a freestanding heterostructure can be used to manipulate the structural and emergent properties of the membrane. In the absence of the strain caused by the substrate, the change in orbital occupancy of the magnetic layer leads to the reorientation of the magnetic easy-axis, that is, perpendicular magnetic anisotropy. These results of designing multiferroic oxide membranes open new avenues to integrate such flexible membranes for electronic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Induced Ferromagnetism in Epitaxial Uranium Dioxide Thin Films

Abstract Actinide materials have various applications that range from nuclear energy to quantum computing. Most current efforts have focused on bulk actinide materials. Tuning functional properties by using strain engineering in epitaxial thin films is largely lacking. Using uranium dioxide (UO 2 ) as a model system, in this work, the authors explore strain engineering in actinide epitaxial thin films and investigate the origin of induced ferromagnetism in an antiferromagnet UO 2 . It is found that UO 2+ x thin films are hypostoichiometric ( x <0) with in‐plane tensile strain, while they are hyperstoichiometric ( x >0) with in‐plane compressive strain. Different from strain engineering in non‐actinide oxide thin films, the epitaxial strain in UO 2 is accommodated by point defects such as vacancies and interstitials due to the low formation energy. Both epitaxial strain and strain relaxation induced point defects such as oxygen/uranium vacancies and oxygen/uranium interstitials can distort magnetic structure and result in magnetic moments. This work reveals the correlation among strain, point defects and ferromagnetism in strain engineered UO 2+ x thin films and the results offer new opportunities to understand the influence of coupled order parameters on the emergent properties of many other actinide thin films.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Structural and Optical Properties of High Entropy (La,Lu,Y,Gd,Ce)AlO 3 Perovskite Thin Films

Mixtures of Ce-doped rare-earth aluminum perovskites are drawing a significant amount of attention as potential scintillating devices. However, the synthesis of complex perovskite systems leads to many challenges. Designing the A-site cations with an equiatomic ratio allows for the stabilization of a single-crystal phase driven by an entropic regime. This work describes the synthesis of a highly epitaxial thin film of configurationally disordered rare-earth aluminum perovskite oxide (La 0.2 Lu 0.2 Y 0.2 Gd 0.2 Ce 0.2 )AlO 3 and characterizes the structural and optical properties. The thin films exhibit three equivalent epitaxial domains having an orthorhombic structure resulting from monoclinic distortion of the perovskite cubic cell. An excitation of 286.5 nm from Gd 3+ and energy transfer to Ce 3+ with 405 nm emission are observed, which represents the potential for high-energy conversion. These experimental results also offer the pathway to tunable optical properties of high-entropy rare-earth epitaxial perovskite films for a range of applications.

36 MATERIALS SCIENCE↗
DOE OSTI2022

In-situ irradiation-induced studies of grain growth kinetics of nanocrystalline UO 2

The thermal conductivity of UO 2 fuel needs to be high enough to dissipate the heat generated from the fission reaction. Since grain size affects thermal conductivity and grain size can evolve with irradiation, it is critical to understand in-reactor UO 2 grain growth. Most studies of grain growth in UO 2 are based on thermally driven processes at elevated temperatures. However, studies have shown that grain growth can occur even at cryogenic temperatures by ballistic processes. Such irradiation-induced grain growth in UO 2 is yet to be studied. Advanced in-situ Kr ion irradiation and transmission electron microscopy were systematically performed on nanocrystalline UO 2 thin films at temperatures ranging from 50 K to 1073 K; grain growth was observed at all temperatures. A combination of manual and machine learning techniques was used to measure and plot grain size evolution against irradiation fluence at various irradiation temperatures. The machine learning method has significantly improved the analysis efficiency and reduced human labors. The grain diameter data were fitted using classical grain growth and thermal spike models to describe grain growth kinetics with and without irradiation effect. Grain growth during low temperature irradiation (≤ 475 K) can be well described by the thermal spike model. Above 475 K, there were additional thermally assisted processes that further accelerate the grain growth. At the highest irradiation temperature about 1075 K, both irradiation-induced dislocation loops and cavities/bubbles were observed to form in the UO 2 . In this report, the effects of irradiation-induced defects on grain growth kinetics are discussed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

High Entropy Oxide Relaxor Ferroelectrics

Relaxor ferroelectrics are important in technological applications due to strong electromechanical response, energy storage capacity, electrocaloric effect, and pyroelectric energy conversion properties. Current efforts to discover and design materials in this class generally rely on substitutional doping as slight changes to local compositional order can significantly affect the Curie temperature, morphotropic phase boundary, and electromechanical responses. In this work, we demonstrate that moving to the strong limit of compositional complexity in an ABO 3 perovskite allows stabilization of relaxor responses that do not rely on a single narrow phase transition region. Entropy-assisted synthesis approaches are utilized to synthesize single-crystal Ba(Ti 0.2 Sn 0.2 Zr 0.2 Hf 0.2 Nb 0.2 )O 3 [Ba(5B)O] films. The high levels of configurational disorder present in this system are found to influence dielectric relaxation, phase transitions, nanopolar domain formation, and Curie temperature. Temperature-dependent dielectric, Raman spectroscopy, and second-harmonic generation measurements reveal multiple phase transitions, a high Curie temperature of 570 K, and the relaxor ferroelectric nature of Ba(5B)O films. The first-principles theory calculations are used to predict possible combinations of cations to design relaxor ferroelectrics and quantify the relative feasibility of synthesizing these highly disordered single-phase perovskite systems. Further, the ability to stabilize single-phase perovskites with various cations on the B-sites offers possibilities for designing high-performance relaxor ferroelectric materials for piezoelectric, pyroelectric, and electrocaloric applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Designing Magnetism in High Entropy Oxides

Abstract In magnetic systems, spin and exchange disorder can provide access to quantum criticality, frustration, and spin dynamics, but broad tunability of these responses and a deeper understanding of strong limit disorder are lacking. Here, it is demonstrated that high entropy oxides present a previously unexplored route to designing materials in which the presence of strong local compositional disorder may be exploited to generate tunable magnetic behaviors—from macroscopically ordered states to frustration‐driven dynamic spin interactions. Single‐crystal La(Cr 0.2 Mn 0.2 Fe 0.2 Co 0.2 Ni 0.2 )O 3 films are used as a model system hosting a magnetic sublattice with a high degree of microstate disorder in the form of site‐to‐site spin and exchange type inhomogeneity. A classical Heisenberg model simplified to represent the highest probability microstates well describes how compositionally disordered systems can paradoxically host magnetic uniformity and demonstrates a path toward continuous control over ordering types and critical temperatures. Model‐predicted materials are synthesized and found to possess an incipient quantum critical point when magnetic ordering types are designed to be in direct competition, this leads to highly controllable exchange bias behaviors previously accessible only in intentionally designed bilayer heterojunctions.

36 MATERIALS SCIENCE↗
DOE OSTI2022

The Role of Oxygen Transfer in Oxide Heterostructures on Functional Properties

A variety of mechanisms are reported to play critical roles in contributing to the high carrier/electron mobility in oxide/SrTiO 3 (STO) heterostructures. By using La 0.95 Sr 0.05 TiO 3 (LSTO) epitaxially grown on different single crystal substrates (such as STO, GdScO 3 , LaAlO 3 , (LaAlO 3 ) 0.3 (Sr 2 AlTaO 6 ) 0.7 , and CeO 2 buffered STO) as the model systems, the formation of a conducting substrate surface layer (CSSL) on STO substrate is shown at relatively low growth temperature and high oxygen pressure (725 °C, 5 × 10 –4 Torr), which contributes to the enhanced conductivity of the LSTO/STO heterostructures. Different from the conventional oxygen vacancy model, this work reveals that the formation of the CSSL occurs when growing an oxide layer (LSTO in this case) on STO, while neither annealing nor the growth of an Au layer alone at the exact same growth condition generates the CSSL in STO. It demonstrates that the oxide layer actively pulls oxygen from STO substrate at given growth conditions, leading to the formation of the CSSL. Here, the observations emphasize the oxygen transfer across film/substrate interface during the synthesis of oxide heterostructures playing a critical role in functional properties.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Effect of lattice strain on magnetism in epitaxial YCrO 3 films

The influence of lattice strain on magnetism is studied for perovskite rare-earth chromite, YCrO 3 (YCO) thin films. A combined theoretical and experimental approach is used to demonstrate the correlation between lattice-strain and magnetic properties of YCO films. The first-principles calculations reveal that the local Cr magnetic moments and the out-of-plane magnetization linearly increase with changing the in-plane lattice strain from compressive to tensile. The experimental results agree with the theory findings showing a strong dependence of magnetization on epitaxial strain in YCO films. These results unveil the lattice-strain-controlled functionalities on perovskite rare-earth chromites and related material systems.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Decoding the shift-invariant data: applications for band-excitation scanning probe microscopy *

A shift-invariant variational autoencoder (shift-VAE) is developed as an unsupervised method for the analysis of spectral data in the presence of shifts along the parameter axis, disentangling the physically-relevant shifts from other latent variables. Using synthetic data sets, we show that the shift-VAE latent variables closely match the ground truth parameters. The shift VAE is extended towards the analysis of band-excitation piezoresponse force microscopy data, disentangling the resonance frequency shifts from the peak shape parameters in a model-free unsupervised manner. The extensions of this approach towards denoising of data and model-free dimensionality reduction in imaging and spectroscopic data are further demonstrated. This approach is universal and can also be extended to analysis of x-ray diffraction, photoluminescence, Raman spectra, and other data sets.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Charge doping effects on magnetic properties of single-crystal La 1-x Sr x (Cr 0.2 Mn 0.2 Fe 0.2 Co 0.2 Ni 0.2 )O 3 (0 ≤ x ≤ 0.5) high-entropy perovskite oxides

The observed influence of hole doping on magnetic properties is mapped for the compositionally complex high-entropy oxide ABO 3 perovskite La 1-x Sr x (Cr 0.2 Mn 0.2 Fe 0.2 Co 0.2 Ni 0.2 )O 3 (0 ≤ x ≤ 0.5). It is found that aliovalent A -site substitution is a viable means to manipulate the magnetically active B -site sublattice. A series of single-crystal films are synthesized and show a general trend toward stronger ferromagnetic response and a shift in magnetic anisotropy as the Sr concentration increases. Magnetometry demonstrates complex and nonuniform responses similar to rigid and uncoupled composites at intermediate dopings. This behavior points to the presence of locally inhomogeneous magnetic phase competition, where ferromagnetic and antiferromagnetic magnetic contributions create a frustrated matrix containing uncompensated spins at the boundaries between these regions. The observations are discussed in the context of known responses to hole doping in the less complex ternary LaT M O 3 (T M =Cr,Mn,Fe,Co,Ni) oxides, and they are found to be different from a simple sum of the doped parents. The results are summarized in a preliminary magnetic phase diagram.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Tuning magnetic and optical properties through strain in epitaxial LaCrO 3 thin films

We report on the effect of epitaxial strain on magnetic and optical properties of perovskite LaCrO 3 (LCO) single crystal thin films. Epitaxial LCO thin films are grown by pulsed laser deposition on proper choice of substrates to impose different strain states. A combined experimental and theoretical approach is used to demonstrate the direct correlation between lattice-strain and functional properties. The magnetization results show that the lattice anisotropy plays a critical role in controlling the magnetic behavior of LCO films. The strain induced tetragonality in the film lattice strongly affects the optical transitions and charge transfer gap in LCO. This study opens possibilities to tailor the functional properties of LCO and related materials by strain engineering in epitaxial growth.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Symmetry mismatch controlled ferroelastic domain ordering and the functional properties of manganite films on cubic miscut substrates

We have studied the magnetotransport properties and strain release mechanisms in ferroelastic La 0.9 Sr 0.1 MnO 3 (LSMO) epitaxial thin films on SrTiO 3 (STO)(001) substrates with different miscut angles. The substrate miscut angle plays a critical role in releasing shear strain and has a huge impact on the properties of the films. The strain relaxes by monoclinic distortion for films on low miscut substrates and for higher miscut substrates, the strain relaxation causes the formation of periodic twin domains with larger periodicities. Furthermore, we observe that the Curie temperature (T C ) decreases systematically, and magnetoresistance (MR) increases with increasing the miscut angle. Such changes in the magnetic and transport properties could be due to the increased density of phase boundaries (PBs) with the increase of miscut angle. This work provides a way to tailor film microstructures and subsequent functional properties of other complex oxide films on miscut substrates with symmetry mismatch.

36 MATERIALS SCIENCE↗