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At least 343 records · Page 19
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Exploring the Spatial Control of Topotactic Phase Transitions Using Vertically Oriented Epitaxial Interfaces

Engineering oxygen vacancy formation and distribution is a powerful route for controlling the oxygen sublattice evolution that affects diverse functional behavior. The controlling of the oxygen vacancy formation process is particularly important for inducing topotactic phase transitions that occur by transformation of the oxygen sublattice. Here we demonstrate an epitaxial nanocomposite approach for exploring the spatial control of topotactic phase transition from a pristine perovskite phase to an oxygen vacancy-ordered brownmillerite (BM) phase in a model oxide La 0.7 Sr 0.3 MnO 3 (LSMO). Incorporating a minority phase NiO in LSMO films creates ultrahigh density of vertically aligned epitaxial interfaces that strongly influence the oxygen vacancy formation and distribution in LSMO. Combined structural characterizations reveal strong interactions between NiO and LSMO across the epitaxial interfaces leading to a topotactic phase transition in LSMO accompanied by significant morphology evolution in NiO. Using the NiO nominal ratio as a single control parameter, we obtain intermediate topotactic nanostructures with distinct distribution of the transformed LSMO-BM phase, which enables systematic tuning of magnetic and electrical transport properties. The use of self-assembled heterostructure interfaces by the epitaxial nanocomposite platform enables more versatile design of topotactic phase structures and correlated functionalities that are sensitive to oxygen vacancies.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Assessing epitaxial regrowth material quality on a micro-transfer printed GaAs substrate

Micro-transfer printing has demonstrated value for device- and array-level heterogeneous integration in a variety of applications. In this report it is used instead to assemble unique substrates with the potential to enable III–V growth templates that are both low-cost and specified at any desired lattice parameter within the range of III–V materials. Critical to this, epitaxial growth crystal quality must be established as comparable to that produced on conventional epi-ready substrates. We demonstrate epitaxial regrowth on gallium arsenide membranes that were transfer printed from their source substrate and onto a target handle. Both morphology and luminescence properties were characterized. Comparing the transfer printed membrane epitaxy with epitaxy on a conventional substrate, we found recombination rates and spatial uniformity from power-dependent photoluminescence and cathodoluminescence, respectively, to yield similar results, suggesting material quality was not adversely limited by the engineered substrate.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Epitaxial columnar growth of strain-free antiferromagnetic Weyl semimetal Mn 3 Sn on wurtzite c -plane GaN/Al 2 O 3 (0001)

Weyl semimetal thin films with excellent crystalline quality are of great interest for antiferromagnetic spintronics. Mn 3 Sn is one Weyl semimetal with great properties and promise for exciting science and applications. It has proven very challenging, however, to grow Mn 3 Sn thin films with smooth surfaces, negligible strain, and excellent crystallinity. In this work, we discuss the successful preparation of epitaxial Mn 3 Sn (0001)-oriented thin films via molecular beam epitaxial growth on c -plane wurtzite GaN which was grown by MBE on Al 2 O 3 (0001). We present the reflection high energy electron diffraction analysis along with x-ray diffraction in order to demonstrate the crystalline quality of the film, and we give atomic models to explain the epitaxial orientation relationships between the crystal lattices of the substrate, GaN layer, and Mn 3 Sn layer. Importantly, we discuss the film lattice parameters as compared to expected values, demonstrating negligible strain both in-plane and out-of-plane . Atomic force microscopy reveals an epitaxial columnar growth mode characterized by flat-top-mesa islands, while scanning tunneling microscopy shows the atomically smooth surfaces of the mesa-top structures. Finally, Rutherford backscattering informs the stoichiometry of the film as well as the layer thicknesses.

Chiral antiferromagnetic material↗
DOE OSTI2013

Epitaxy of Zn{sub 2}TiO{sub 4} (1 1 1) thin films on GaN (0 0 1)

Highlights: ► High-permittivity spinel Zn{sub 2}TiO{sub 4} thin films were grown on GaN (0 0 1) by sputtering. ► Oxygen atmosphere and post heat-treatment annealing effectively enhanced epitaxy. ► The epitaxial Zn{sub 2}TiO{sub 4} modifies the dielectric properties of ceramic oxide. - Abstract: High-permittivity spinel Zn{sub 2}TiO{sub 4} thin films were grown on GaN (0 0 1) by rf-sputtering. Grazing-angle, powder, and pole-figure X-ray diffractometries (XRD) were performed to identify the crystallinity and the preferred orientation of the Zn{sub 2}TiO{sub 4} films. Lattice image at the Zn{sub 2}TiO{sub 4} (1 1 1)/GaN (0 0 1) interface was obtained by high-resolution transmission-electron microscopy (HR-TEM). An oxygen atmosphere in sputtering and post heat-treatment using rapid thermal annealing effectively enhanced the epitaxy. The epitaxial relationship was determined from the XRD and HR-TEM results: (111){sub Zn{sub 2TiO{sub 4}}}||(001){sub GaN}, (202{sup ¯}){sub Zn{sub 2TiO{sub 4}}}||(110){sub GaN},and[21{sup ¯}1{sup ¯}]{sub Zn{sub 2TiO{sub 4}}}||[01{sup ¯}10]{sub GaN}. Finally, the relative permittivity, interfacial trap density and the flat-band voltage of the Zn{sub 2}TiO{sub 4} based capacitor were ∼18.9, 8.38 × 10{sup 11} eV{sup −1} cm{sup −2}, and 1.1 V, respectively, indicating the potential applications of the Zn{sub 2}TiO{sub 4} thin film to the GaN-based metal-oxide-semiconductor capacitor.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Lattice-Mismatched van der Waals Epitaxy and Photoluminescence of Two-Dimensional GaxIn1-xSe Alloys on Si(111)

GaxIn1-xSe (GIS) alloys are two-dimensional (2D) layered materials with band gaps and lattice parameters of interest for many energy and electronic applications. They can be fabricated using van der Waals epitaxy, which is an emerging technique that offers unprecedented opportunities for 2D optoelectronic devices and epitaxy processes. This work has demonstrated van der Waals epitaxy of GIS alloys for the first time. Films with x compositions of 0, 0.062, 0.164, 0.680, 0.894, and 1 and tunable lattice constants were grown on Si(111) substrates, and characterized by X-ray diffraction pole figure and transmission electron microscope analysis. In spite of the lattice mismatches (InSe is 4.1% too large and GaSe is 2.8% too small), these alloys grow epitaxially, with Si(111) || GIS(001) and Si[1-10] || GIS[100] orientation. Photoluminescence was used to measure tunable band gaps in the absorber-relevant 1.3-2.0 eV range as a function of x composition and showed GIS did not degrade after capping with Se and prolonged storage. Therefore, GIS alloys exhibit a technologically advantageous combination of tunable band gap and photoluminescence with relaxed lattice parameter and rotational registry with the substrate.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Growth and Characterization of Epitaxial FeWO 4 Thin Films with Controlled Oxygen Stoichiometry

Here, we report the growth of single-phase epitaxial FeWO 4 thin films, using plasma-assisted molecular beam epitaxy, and investigate structural, optical, and electronic properties. The FeWO 4 films grow in (100) orientation on c-plane sapphire (0001) substrates and exhibit 3 rotational twin variants where FeWO 4 [001] is aligned to sapphire [100] equivalent in-plane directions. X-ray diffraction measurements indicate that the epitaxial FeWO 4 (100) structure is optimized when 80-100 W of rf power is applied to an atomic oxygen source during growth, yielding films with minimal strain and impurity phases or other orientations. In films grown with 120 W of rf power, FeWO 4 crystallites develop inhomogeneous and homogeneous strains and are potentially contaminated with Fe 3+ oxide phase impurities. In films grown with 60 W of rf power, FeWO 4 crystallites do not form fully epitaxial layers. X-ray photoelectron spectroscopy indicates that the structural changes are correlated with the Fe 3+ /Fe 2+ oxidation state ratio increasing from 0.6-1.4 with rf power from 60-120 W. X-ray fluorescence spectroscopy indicates that the Fe/W composition ratio is also increasing from 1.1-1.8 with rf power from 60-120 W. Ultraviolet and visible optical absorption spectra indicate a 1.8 ± 0.1 eV band gap with an additional interband absorption feature at 3.1 ± 0.1 eV in the 80-100 W films, with similar onsets observed in the 60 W films. In the 120 W films, the higher lying transition is shifted to 2.7 ± 0.1 eV due to the Fe 3+ enrichment. Electrical resistivity decreases over 2 orders of magnitude with oxidation from 10 4 -10 5 Ω cm in 60 W films to 120 ± 10 Ω cm in 120 W films. Thermopower measurements show p-type to n-type conductivity conversion when oxidation states shift from Fe 2+ majority in the 100 W films to Fe 3+ majority in the 120 W films. We conclude that electron polaron hopping driven by Fe 3+ is a dominant transport mechanism and a source of n-type conductivity in overoxidized FeWO 4 films.

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

Spontaneous Lithiation of Binary Oxides during Epitaxial Growth on LiCoO 2

Epitaxial growth is a powerful tool for synthesizing heterostructures and integrating multiple functionalities. Interfacial mixing can readily occur at temperatures required for complete film crystallization and can significantly modify the properties of layered structures, particularly for those containing energy storage materials with smaller cations. Here we show a two-step sequence involving the growth of an epitaxial LiCoO 2 cathode layer followed by the deposition of a binary transition metal oxide (WO 3 , TiO 2 , and others) in which controlled lithiation of the binary oxide occurs. Orientation-controlled epitaxial synthesis of the model solid-state-electrolyte Li 2 WO 4 and model anode material Li 4 Ti 5 O 12 occurs as WO 3 and TiO 2 nucleate their respective host lattices and attract Li ions from the underlying cathode. The cathode layer readily provides a tunable amount of Li ions for the controlled lithiation of the subsequent layer. We demonstrate that this approach can be used for energy materials discovery and exploring different combinations of epitaxial interfaces that can serve as well-defined model systems for mechanistic studies of energy storage and conversion processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Photon Transport in One-Dimensional Incommensurately Epitaxial CsPbX 3 Arrays

One-dimensional nanoscale epitaxial arrays serve as a great model in studying fundamental physics and for emerging applications. With an increasing focus laid on the Cs-based inorganic halide perovskite out of its outstanding material stability, we have applied vapor phase epitaxy to grow well aligned horizontal CsPbX 3 (X: Cl, Br, or I or their mixed) nanowire arrays in large scale on mica substrate. The as-grown nanowire features a triangular prism morphology with typical length ranging from a few tens of micrometers to a few millimeters. Structural analysis reveals that the wire arrays follow the symmetry of mica substrate through incommensurate epitaxy, paving a way for a universally applicable method to grow a broad family of halide perovskite materials. We have studied the unique photon transport in the one-dimensional structure in the all-inorganic Cs-based perovskite wires via temperature dependent and spatially resolved photoluminescence. Furthermore, epitaxy of well oriented wire arrays in halide perovskite would be a promising direction for enabling the circuit-level applications of halide perovskite in high-performance electro-optics and optoelectronics.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Twin-Domain Formation in Epitaxial Triangular Lattice Delafossites

Twin domains are often found as structural defects in symmetry mismatched epitaxial thin films. The delafossite ABO 2 , which has a rhombohedral structure, is a good example that often forms twin domains. Although bulk metallic delafossites are known to be the most conducting oxides, high conductivity is yet to be realized in thin film forms. Suppressed conductivity found in thin films is mainly caused by the formation of twin domains, and their boundaries can be a source of scattering centers for charge carriers. To overcome this challenge, the underlying mechanism for their formation must be understood so that such defects can be controlled and eliminated. Here, we report the origin of structural twins formed in a CuCrO 2 delafossite thin film on a substrate with hexagonal or triangular symmetries. A robust heteroepitaxial relationship is found for the delafossite film with the substrate, and the surface termination turns out to be critical to determine and control the domain structure of epitaxial delafossites. Based on such discoveries, we also demonstrate twin-free epitaxial thin films grown on high-miscut substrates. Finally, this finding provides an important synthesis strategy for growing single-domain delafossite thin films and can be applied to other delafossites for the epitaxial synthesis of high-quality thin films.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Orientation-Controlled Large-Area Epitaxial PbI 2 Thin Films with Tunable Optical Properties

Lead iodide (PbI 2 ) as a layered material has emerged as an excellent candidate for optoelectronics in the visible and ultraviolet regime. Micrometer-sized flakes synthesized by mechanical exfoliation from bulk crystals or by physical vapor deposition have shown a plethora of applications from low-threshold lasing at room temperature to high-performance photodetectors with large responsivity and faster response. However, large-area centimeter-sized growth of epitaxial thin films of PbI 2 with well-controlled orientation has been challenging. Additionally, the nature of grain boundaries in epitaxial thin films of PbI 2 remains elusive. Here, we use mica as a model substrate to unravel the growth mechanism of large-area epitaxial PbI 2 thin films. The partial growth leading to uncoalesced domains reveals the existence of inversion domain boundaries in epitaxial PbI 2 thin films on mica. Combining the experimental results with first-principles calculations, we also develop an understanding of the thermodynamic and kinetic factors that govern the growth mechanism, which paves the way for the synthesis of high-quality large-area PbI 2 on other substrates and heterostructures of PbI 2 on single-crystalline graphene. Here, the ability to reproducibly synthesize high-quality large-area thin films with precise control over orientation and tunable optical properties could open up unique and hitherto unavailable opportunities for the use of PbI 2 and its heterostructures in optoelectronics, twistronics, substrate engineering, and strain engineering.

2D materials↗
DOE OSTI2024

Nanoscale Control of Intrinsic Magnetic Topological Insulator MnBi 2 Te 4 Using Molecular Beam Epitaxy: Implications for Defect Control

Intrinsic magnetic topological insulators have emerged as a promising platform to study the interplay between the topological surface states and ferromagnetism. This unique interplay can give rise to a variety of exotic quantum phenomena, including the quantum anomalous Hall effect and axion insulating states. Here, in this study, utilizing molecular beam epitaxy (MBE), we present a comprehensive study of the growth of MnBi 2 Te 4 thin films on Si (111), epitaxial graphene, and highly ordered pyrolytic graphite substrates. By combining a suite of in situ characterization techniques, we obtain critical insights into the nanoscale control of MnBi 2 Te 4 epitaxial growth. First, we extract the free energy landscape for the epitaxial relationship as a function of the in-plane angular distribution. Then, by employing an optimized layer-by-layer growth, we determine the chemical potential and Dirac point of the thin film at different thicknesses and how this quantity is manifested by the dopant compensation from different antisite defects. Overall, these results establish a foundation for understanding the growth kinetics of MnBi 2 Te 4 and pave the way for future applications of MBE-grown thin films in emerging topological quantum materials.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Density Functional Theory Study of Epitaxially Strained Monolayer Transition Metal Chalcogenides for Piezoelectricity Generation

Two-dimensional transition metal chalcogenides (2D TMCs) are known for their wide range of bandgaps, flexibility, and high strength. Recent synthesis and data mining efforts indicate that 56 2D TMCs have low exfoliation energies and are relatively stable in monolayer form. Under epitaxial strain, we predict using density functional theory (DFT) calculations that the majority of these 2D TMCs can accommodate ±10% strain without breaking their crystal symmetry. The elastic and piezoelectric tensors indicate that 22 of 56 candidates are piezoelectric, and we derive their in-plane piezoelectric coefficient d 11 . The epitaxial strain is further predicted to enhance the d 11 by over 100% at 10% tensile epitaxial strain for most of these piezoelectric 2D TMCs. ReSe 2 at pristine state and Au 2 Se 2 at +5% epitaxial strain are predicted to obtain the extreme d 11 coefficients at -120 and 326 pm/V, respectively. Lastly, these findings have implications for the use of high-performance 2D piezoelectric materials in devices.

2D materials↗
DOE OSTI2022

Fabrication of a Microcavity Prepared by Remote Epitaxy over Monolayer Molybdenum Disulfide

We report advances in epitaxy have enabled the preparation of high-quality material architectures consisting of incommensurate components. Remote epitaxy based on lattice transparency of atomically thin graphene has been intensively studied for cost-effective advanced device manufacturing and heterostructure formation. However, remote epitaxy on nongraphene two-dimensional (2D) materials has rarely been studied even though it has a broad and immediate impact on various disciplines, such as many-body physics and the design of advanced devices. Herein, we report remote epitaxy of ZnO on monolayer MoS 2 and the realization of a whispering-gallery-mode (WGM) cavity composed of a single crystalline ZnO nanorod and monolayer MoS 2 . Cross-sectional transmission electron microscopy and first-principles calculations revealed that the nongraphene 2D material interacted with overgrown and substrate layers and also exhibited lattice transparency. The WGM cavity embedding monolayer MoS 2 showed enhanced luminescence of MoS 2 and multimodal emission.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Atomic-Scale Insights into the Lateral and Vertical Epitaxial Growth in Two-Dimensional Pd 2 Se 3 –MoS 2 Heterostructures

Two-dimensional (2D) materials form heterostructures in both the lateral and vertical directions when two different materials are interfaced, but with totally different bonding mechanisms of covalent in-plane to van der Waal’s layered interactions. Understanding how the competition between lateral and vertical forces influences the epitaxial growth is important for future materials development of complex mixed layered heterostructures. In this study, we use atomic-resolution annular dark-field scanning transmission electron microscopy to study the detailed atomic arrangements at mixed 2D heterostructure interfaces composed of two semiconductors with distinctly different crystal symmetry and elemental composition, Pd 2 Se 3 :MoS 2 , in order to understand the role of different chemical bonds on the resultant epitaxy. Pd 2 Se 3 is grown off the step edge in bilayer MoS 2 , and the vertical and lateral epitaxial relationships of the Pd 2 Se 3 –MoS 2 heterostructures are investigated. We find that the similarity of geometry at the interface with one metal (Pd or Mo) atoms bonded with two chalcogens (S or Se) are the crucial factors to make the atomically stitched lateral junction of 2D heterostructures. In addition, the vertical van der Waal interactions that are normally dominant in layered materials can be overcome by in-plane forces if the interfacial atomic stitching is high in quality and low in defect density. This knowledge should help guide the approaches for improving the epitaxy in mixed 2D heterostructures and seamless stitching of in-plane 2D heterostructures with various complex monolayer structures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Structure Prediction of Ionic Epitaxial Interfaces with Ogre Demonstrated for Colloidal Heterostructures of Lead Halide Perovskites

Colloidal epitaxial heterostructures are nanoparticles composed of two different materials connected at an interface, which can exhibit properties different from those of their individual components. Combining dissimilar materials offers exciting opportunities to create a wide variety of functional heterostructures. However, assessing structural compatibility–the main prerequisite for epitaxial growth–is challenging when pairing complex materials with different lattice parameters and crystal structures. This complicates both the selection of target heterostructures for synthesis and the assignment of interface models when new heterostructures are obtained. Here, we demonstrate Ogre as a powerful tool to accelerate the design and characterization of colloidal heterostructures. To this end, we implemented developments tailored for the high-efficiency prediction of epitaxial interfaces between ionic/polar materials, which encompass most colloidal semiconductors. These include the use of pre-screening candidate models based on charge balance at the interface and the use of a classical potential for fast energy evaluations, with parameters automatically calculated based on the input bulk structures. These developments are validated for perovskite-based CsPbBr 3 /Pb 4 S 3 Br 2 heterostructures, where Ogre produces interface models in excellent agreement with density functional theory and experiments. Furthermore, we use Ogre to rationalize the templating effect of CsPbCl 3 on the growth of lead sulfochlorides, where perovskite seeds induce the formation of Pb 4 S 3 Cl 2 rather than Pb 3 S 2 Cl 2 due to better epitaxial compatibility. Finally, combining Ogre simulations with experimental data enables us to unravel the structure and composition of the hitherto unsolved CsPbBr 3 /Bi x Pb y S z interface, and to assign a structure to several other reported metal halide- and oxide-based interfaces. The Ogre package is available on GitHub or via the OgreInterface desktop application, available for Windows, Linux, and Mac.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Van der Waals epitaxial growth of two-dimensional single-crystalline GaSe domains on graphene

Two-dimensional (2D) van der Waals (vdW) heterostructures are a family of artificially-structured materials that promise tunable optoelectronic properties for devices with enhanced functionalities. Compared to stamping, direct epitaxy of vdW heterostructures is ideal for clean interlayer interfaces and scalable device fabrication. Here, we explore the synthesis and preferred orientations of 2D GaSe atomic layers on graphene (Gr) by vdW epitaxy. Guided by the wrinkles on graphene, GaSe nuclei form that share a predominant lattice orientation. Due to vdW epitaxial growth many nuclei grow as perfectly aligned crystals and coalesce to form large (tens of microns), single-crystal flakes. Through theoretical investigations of interlayer energetics, and measurements of preferred orientations by atomic-resolution STEM and electron diffraction, a 10.9 interlayer rotation of the GaSe lattice with respect to the underlying graphene is found to be the most energetically preferred vdW heterostructure with the largest binding energy and the longest-range ordering. These GaSe/Gr vdW heterostructures exhibit an enhanced Raman E 2 1g band of monolayer GaSe along with highly-quenched photoluminescence due to strong charge transfer. Despite the very large lattice mismatch of GaSe/Gr through vdW epitaxy, the predominant orientation control and convergent formation of large single-crystal flakes demonstrated here is promising for the scalable synthesis of large-area vdW heterostructures for the development of new optical and optoelectronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2011

Azimuthal reflection high-energy electron diffraction study of MnAs growth on GaAs(001) by molecular beam epitaxy

Azimuthal reflection high-energy electron diffraction (ARHEED) and in situ grazing incidence synchrotron x-ray diffraction techniques are employed to investigate the growth, epitaxial orientation, and interfacial structure of MnAs layers grown on GaAs(001) by molecular beam epitaxy (MBE). We demonstrate the power and reliability of ARHEED scans as a routine tool in characterizing the formation of epitaxial films. The ARHEED scans clearly reveal the formation of the rectangular MnAs unit cell during growth on GaAs(001) for a MnAs layer thickness of 2.1 {+-} 0.2 monolayers with a tensile strain along the MnAs[1120] direction. A periodic coincidence site lattice, which is known to form along the MnAs [0001] direction to release the strain due to the huge lattice mismatch ({approx}30%) also produces periodic satellites of the diffraction spots in the ARHEED scan. The formation of different epitaxial orientations of MnAs during MBE growth can be directly observed using ARHEED scans. ARHEED is demonstrated to have a resolution similar to synchrotron x-ray diffraction with a double crystal monochromator, yielding full width at half maximum values of reflections as small as 0.005 reciprocal lattice units.

36 MATERIALS SCIENCE↗
DOE OSTI2011

Suppression of planar defects in the molecular beam epitaxy of GaAs/ErAs/GaAs heterostructures

We present a growth method that overcomes the mismatch in rotational symmetry of ErAs and conventional III-V semiconductors, allowing for epitaxially integrated semimetal/semiconductor heterostructures. Transmission electron microscopy and reflection high-energy electron diffraction reveal defect-free overgrowth of ErAs layers, consisting of >2x the total amount of ErAs that can be embedded with conventional layer-by-layer growth methods. We utilize epitaxial ErAs nanoparticles, overgrown with GaAs, as a seed to grow full films of ErAs. Growth proceeds by diffusion of erbium atoms through the GaAs spacer, which remains registered to the underlying substrate, preventing planar defect formation during subsequent GaAs growth. This growth method is promising for metal/semiconductor heterostructures that serve as embedded Ohmic contacts to epitaxial layers and epitaxially integrated active plasmonic devices.

36 MATERIALS SCIENCE↗