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At least 595 records · Page 33
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

Influence of the interfacing with an electrically inhomogeneous bottom electrode on the ferroelectric properties of epitaxial PbTiO3

The influence of an electrically inhomogeneous epitaxial bottom layer on the ferroelectric and electrical properties has been explored in epitaxial PbTiO3 (PTO)/La0.7Sr0.3MnO3 (LSMO) submicron structures using atomic force microscopy. The submicron LSMO-dot structures underneath the ferroelectric PTO film allow exploring gradual changes in material properties. The LSMO interfacial layer influences significantly both electrical and ferroelectric properties of the upper PTO layer. The obtained results show that the as-grown polarization state of an epitaxial ferroelectric layer is strongly influenced by the properties of the layer on top of which it is deposited.

Kim, Yunseok↗
DOE OSTI2014

Epitaxial polymorphism of La{sub 2}O{sub 3} on Si(111) studied by in situ x-ray diffraction

The phase formation of La{sub 2}O{sub 3} epitaxial films during growth on Si(111) is investigated by synchrotron-based in situ grazing incidence x-ray diffraction and high resolution transmission electron microscopy. We find that first a 2–4 nm thick cubic bixbyite La{sub 2}O{sub 3} layer grows at the interface to Si(111) substrate, followed by a hexagonal La{sub 2}O{sub 3} film. Hence, to keep a cubic on cubic heteroepitaxy and to achieve high quality epitaxial nanostructures or multi-layers, the thickness of the interfacial La{sub 2}O{sub 3} layer has to be restricted to 2 nm. The larger formation energy of the cubic phase can only partially be compensated by the biaxial strain in the epitaxial film based on density functional perturbation theory. Hence, the stabilization of the cubic phase is not due to bulk strain but could be related to a lower surface or interface free energy, or to kinetic effects.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Growth of ferroelectric Ba{sub 0.8}Sr{sub 0.2}TiO{sub 3} epitaxial films by ultraviolet pulsed laser irradiation of chemical solution derived precursor layers

Highly crystalline epitaxial Ba{sub 0.8}Sr{sub 0.2}TiO{sub 3} (BST) thin-films are grown on (001)-oriented LaNiO{sub 3}-buffered LaAlO{sub 3} substrates by pulsed laser irradiation of solution derived barium-zirconium-titanium precursor layers using a UV Nd:YAG laser source at atmospheric conditions. The structural analyses of the obtained films, studied by X-ray diffractometry and transmission electron microscopy, demonstrate that laser processing allows the growth of tens of nm-thick BST epitaxial films with crystalline structure similar to that of films obtained through conventional thermal annealing methods. However, the fast pulsed nature of the laser employed leads to crystallization kinetic evolution orders of magnitude faster than in thermal treatments. The combination of specific photothermal and photochemical mechanisms is the main responsible for the ultrafast epitaxial laser-induced crystallization. Piezoresponse microscopy measurements demonstrate equivalent ferroelectric behavior in laser and thermally annealed films, being the piezoelectric constant ∼25 pm V{sup −1}.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Incorporation of indium on cubic GaN epitaxially induced on a nanofaceted Si(001) substrate by phase transition

Here, the incorporation of In on the non-polar, piezoelectric-free (001) facet of cubic (c-) GaN epitaxially grown over a Si(001) substrate by metal-organic vapor phase epitaxy is reported. Relying on a hexagonal (h-) to c-phase transformation during epitaxy on an 800 nm-wide, Si(111)-faceted v-groove patterned into the substrate, the GaN epilayer at cross sectional view retains a triangular c-phase inside a chevron-shaped h-phase that results in a top surface bounded by a (001) facet parallel to Si(001) at the center and (11¯01) facets at both edges. A stack of five, ~3 nm-thick, In x Ga 1–x N/GaN quantum wells (QWs) was deposited on the double-phased top surface. The c-phase region up to the QWs keeps extremely small misfit (~0.002) to the fully relaxed h-GaN underneath it and is in tensile stress implying undefected by the h-c phase interface. Lastly, the In incorporation on a strained non-polar (001) of c-GaN is comparable with that on totally relaxed semi-polar (11¯01) of h-GaN without noticeable adatom migration across the phase boundary, and sufficient to provide the room-temperature green emission at 496 nm from the c-In x Ga 1–x N/GaN QWs on Si(001) in photoluminescence.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Exposing high-energy surfaces by rapid-anneal solid phase epitaxy

The functional design of nanoscale transition metal oxide heterostructures depends critically on the growth of atomically flat epitaxial thin films. Much of the time, improved functionality is expected for heterostructures and surfaces with orientations that do not have the lowest surface free energy. For example, crystal faces with a high surface free energy, such as rutile (001) planes, frequently exhibit higher catalytic activities but are correspondingly harder to synthesize due to energy-lowering faceting transitions. We propose a broadly applicable rapid-anneal solid phase epitaxial synthesis approach for the creation of atomically flat, high surface free energy oxide heterostructures. We also demonstrate its efficacy via the synthesis of atomically flat, epitaxial RuO 2 (001) films with a superior oxygen evolution activity, quantified by their lower onset potential and higher current density, relative to that of more common RuO 2 (110) films.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2018

Low magnetic damping and large negative anisotropic magnetoresistance in half-metallic Co 2-x Mn 1+x Si Heusler alloy films grown by molecular beam epitaxy

Co 2-x Mn 1+x Si films with various composition x were epitaxially grown using molecular beam epitaxy (MBE). High crystallinity and atomic ordering in the prepared Co 2-x Mn 1+x Si films were observed, and their magnetic damping and anisotropic magnetoresistance (AMR) effect were systematically investigated. An ultra-low magnetic damping constant of 0.0007 was obtained in the Co 2-x Mn 1+x Si film with a valence electron number (NV) of about 29.0. Additionally, a relatively large negative AMR effect was observed in the Co 2-x Mn 1+x Si films that had a N V of about 29.0. This low damping and the large negative AMR effect indicate that epitaxial Co 2-x Mn 1+x Si films with high atomic ordering grown by MBE possess a high-spin polarization. Half-metals have potential for enhancing the performance of various kinds of spintronic devices, such as magnetic sensors and magnetic random access memory (MRAM) devices, because the conduction electrons are completely spin-polarized due to the Fermi level (EF) being in the energy gap of one of the spin channels. Among the half-metals, Co-based Heusler alloys are expected to show half-metallic properties at room temperature due to their high Curie temperature. In the past decade, high tunnel magnetoresistance (TMR) and current-perpendicular-to-plane giant magnetoresistance (CPP-GMR) have been experimentally demonstrated using Co-based Heusler alloy electrodes. Furthermore, further improvement of their half-metallic properties is required to obtain improved performance in magnetic tunnel junctions (MTJs) and CPP-GMR devices.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Epitaxial integration and properties of SrRuO 3 on silicon

We report the integration of SrRuO 3 , one of the most widely used oxide electrode materials in functional oxide heterostructures, with silicon using molecular-beam epitaxy and an SrTiO 3 buffer layer. The resulting SrRuO 3 film has a rocking curve full width at half maximum of 0.01°, a resistivity at room temperature of 250 μΩ cm, a residual resistivity ratio (ρ 300 K/ρ 4 K) of 11, and a paramagnetic-to-ferromagnetic transition temperature of ~160 K. These structural, electrical, and magnetic properties compare favorably to the best reported values for SrRuO 3 films on silicon and rival those of epitaxial SrRuO 3 films produced directly on SrTiO 3 single crystals by thin film growth techniques other than molecular-beam epitaxy. These high quality SrRuO 3 films with metallic conductivity on silicon are relevant to integrating multi-functional oxides with the workhorse of semiconductor technology, silicon.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Electronic structure of epitaxially grown and regrown GaN pn junctions characterized by scanning Kelvin probe and capacitance microscopy

Epitaxial regrowth of GaN pn junctions is a key technology for realization of a variety of high-performance GaN power electronic devices. However, the regrowth process can introduce impurities and defects that degrade a device’s performance. Here, we show that scanning Kelvin probe force microscopy and scanning capacitance microscopy can be used in a cross-sectional geometry to probe dopant distributions and an electronic structure in epitaxially grown GaN pn junctions. These measurements enable profiling of potential and dopant distributions across GaN pn junctions produced by uninterrupted epitaxial growth and by regrowth on an etched surface. Clear differences are observed in comparisons to the electronic structure of these two types of junctions that can be correlated with results of complementary characterization of dopant distributions reported for similarly grown structures. These measurements also suggest the presence of defects in etch-and-regrow pn junction structures that extend nearly 1 μm below the regrown interface.

Kim, Tae-Hyeon (ORCID:0000000341530617)↗
DOE OSTI2022

Synthesis of antiferromagnetic Weyl semimetal Mn 3 Ge on insulating substrates by electron beam assisted molecular beam epitaxy

The antiferromagnetic kagome semimetals Mn 3 X (X = Ge, Sn, Ga) are of great interest due to properties arising from their Berry curvature, such as large anomalous Nernst and anomalous Hall coefficients, and spin to charge conversion efficiencies at ambient temperatures. However, the synthesis of epitaxial thin films of Mn 3 Ge in the desired hexagonal phase has been challenging because they do not wet insulating substrates, necessitating the use of a metallic buffer layer. Furthermore, a ferrimagnetic tetragonal phase also forms readily under typical growth conditions, interfering with hexagonal phase properties. We have synthesized atomically smooth and continuous epitaxial thin films of hexagonal Mn 3 Ge directly on insulating LaAlO 3 (111) substrates using electron beam assisted molecular beam epitaxy, using a three-step process that mitigates the formation of the tetragonal phase. The anomalous Nernst coefficient is found to be more than six times larger in our films than in sputtered thin films of Mn 3 Ge and significantly larger than that of Fe. Our approach can be used to grow thin layers of kagome materials, without interference from a buffer layer in transport properties, and may be applicable to a broader range of materials with large surface energies that do not grow readily on insulating substrates.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Two-level systems in nucleated and non-nucleated epitaxial alpha-tantalum films

Building usefully coherent superconducting quantum processors depends on reducing losses in their constituent materials. Tantalum, like niobium, has proven utility as the primary superconducting layer within highly coherent qubits. However, unlike Nb, high temperatures are typically used to stabilize the desirable body-centered-cubic phase, α-Ta, during thin film deposition. It has long been known that a thin Nb layer permits the room-temperature nucleation of α-Ta, but here we observe the epitaxial process and present few-photon microwave loss measurements in Nb-nucleated Ta films. We compare resonators patterned from Ta films grown at high temperature (500 °C) and films nucleated at room temperature, in order to understand the impact of the crystalline order on quantum coherence. In both cases, films grew with Al 2 O 3 (001) ∥ Ta (110), indicating that the epitaxial orientation is independent of temperature and is preserved across the Nb/Ta interface. We use conventional low-power spectroscopy to measure two level system (TLS) loss as well as an electric-field bias technique to measure the effective dipole moments of TLS in the surfaces of resonators. In our measurements, Nb-nucleated Ta resonators had greater loss tangent (1.5 ± 0.1 × 10 -5 ) than non-nucleated (5 ± 1× 10 -6 ) in approximate proportion to defect densities as characterized by x-ray diffraction (0.27° vs 0.18° [110] reflection width) and electron microscopy (30 vs 70 nm domain size). Furthermore, the dependence of the loss tangent on domain size indicates that the development of more ordered Ta films is likely to lead to improvements in qubit coherence times. Moreover, low-temperature α-Ta epitaxy may enable the growth of microstate-free heterostructures, which would not withstand high temperature processing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Ferroelectric AlBN films by molecular beam epitaxy

We report the properties of molecular beam epitaxy deposited AlBN thin films on a recently developed epitaxial nitride metal electrode, Nb2N. While a control AlN thin film exhibits standard capacitive behavior, distinct ferroelectric switching is observed in the AlBN films with increasing Boron mole fraction. The measured remnant polarization Pr∼15μC/cm2 and coercive field Ec∼ 1.45 MV/cm in these films are smaller than those recently reported on films deposited by sputtering, due to incomplete wake-up, limited by current leakage. Because AlBN preserves the ultrawide energy bandgap of AlN compared to other nitride hi-K dielectrics and ferroelectrics, and it can be epitaxially integrated with GaN and AlN semiconductors, its development will enable several opportunities for unique electronic, photonic, and memory devices.

Physics↗
DOE OSTI2011

Tailoring a two-dimensional electron gas at the LaAlO{sub 3}/SrTiO{sub 3} (001) interface by epitaxial strain.

Recently a metallic state was discovered at the interface between insulating oxides, most notably LaAlO{sub 3} and SrTiO{sub 3}. Properties of this two-dimensional electron gas (2DEG) have attracted significant interest due to its potential applications in nanoelectronics. Control over this carrier density and mobility of the 2DEG is essential for applications of these unique systems, and may be achieved by epitaxial strain. However, despite the rich nature of strain effects on oxide materials properties, such as ferroelectricity, magnetism, and superconductivity, the relationship between the strain and electrical properties of the 2DEG at the LaAlO{sub 3}/SrTiO{sub 3} heterointerface remains largely unexplored. Here, we use different lattice constant single-crystal substrates to produce LaAlO{sub 3}/SrTiO{sub 3} interfaces with controlled levels of biaxial epitaxial strain. We have found that tensile-strained SrTiO{sub 3} destroys the conducting 2DEG, while compressively strained SrTiO{sub 3} retains the 2DEG, but with a carrier concentration reduced in comparison to the unstrained LaAlO{sub 3}/SrTiO{sub 3} interface. We have also found that the critical LaAlO{sub 3} overlayer thickness for 2DEG formation increases with SrTiO{sub 3} compressive strain. Our first-principles calculations suggest that a strain-induced electric polarization in the SrTiO{sub 3} layer is responsible for this behavior. The polarization is directed away from the interface and hence creates a negative polarization charge opposing that of the polar LaAlO{sub 3} layer. This behavior both increases the critical thickness of the LaAlO{sub 3} layer, and reduces carrier concentration above the critical thickness, in agreement with our experimental results. Our findings suggest that epitaxial strain can be used to tailor 2DEGs properties of the LaAlO{sub 3}/SrTiO{sub 3} heterointerface.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Metallicity and anomalous Hall effect in epitaxially strained, atomically thin RuO 2 films

The anomalous Hall effect (AHE), a hallmark of time-reversal symmetry breaking, has been reported in rutile RuO 2 , a debated metallic altermagnetic candidate. Previously, AHE in RuO 2 was observed only in strain-relaxed thick films under extremely high magnetic fields (~50 T). Yet, in ultrathin strained films with distinctive anisotropic electronic structures, there are no reports, likely due to disorder and defects suppressing metallicity thus hindering its detection. Here, we demonstrate that ultrathin, fully strained 2 nm TiO 2 /t nm RuO 2 /TiO 2 (110) heterostructures, grown by hybrid molecular beam epitaxy, retain metallicity and exhibit a sizeable AHE at a significantly lower magnetic field (< 9 T). Density functional theory calculations reveal that epitaxial strain stabilizes a noncompensated magnetic ground state and reconfigures magnetic ordering in RuO 2 (110) thin films. These findings establish ultrathin RuO 2 as a platform for strain-engineered magnetism and underscore the transformative potential of epitaxial design in advancing spintronic technologies.

MBE↗
DOE OSTI2026

Altermagnetic polar metallic phase in ultrathin epitaxially strained RuO 2 films

Altermagnetism refers to a wide class of magnetic orders featuring magnetic sublattices with opposite spins related by rotational symmetries, resulting in nontrivial spin splitting and magnetic multipoles. However, the direct observation of the altermagnetic transition remains elusive. Here, by combining theoretical analysis, electrical transport, X-ray, and optical spectroscopies, we establish a phase diagram in hybrid molecular beam epitaxy-grown RuO 2 /TiO 2 (110) films, mapping symmetries along with altermagnetic/electronic/structural phase transitions as functions of film thickness and temperature. This features an altermagnetic metallic polar phase in epitaxially strained 2 nm films, suggesting a potential link between polar metals and altermagnetic materials. Such a clear signature of a magnetic phase transition at ~500 K is observed exclusively in ultrathin strained films, unlike in bulk RuO 2 single crystals. These results highlight the power of epitaxial heterostructure engineering to induce altermagnetism in systems initially nonmagnetic, opening avenues for realizing emergent quantum phases with multifunctional properties.

RuO2 thin film↗
DOE OSTI2016

Structural phase diagram for ultra-thin epitaxial Fe 3 O 4 / MgO(0 01) films: thickness and oxygen pressure dependence

A systematic investigation of the thickness and oxygen pressure dependence for the structural properties of ultra-thin epitaxial magnetite (Fe 3 O 4 ) films has been carried out; for such films, the structural properties generally differ from those for the bulk when the thickness ≤10 nm. Iron oxide ultra-thin films with thicknesses varying from 3 nm to 20 nm were grown on MgO (001) substrates using molecular beam epitaxy under different oxygen pressures ranging from 1 × 10 -7 torr to 1 × 10 -5 torr. The crystallographic and electronic structures of the films were characterized using low energy electron diffraction (LEED) and x-ray photoemission spectroscopy (XPS), respectively. Moreover, the quality of the epitaxial Fe 3 O 4 ultra-thin films was judged by magnetic measurements of the Verwey transition, along with complementary XPS spectra. We observed that under the same growth conditions the stoichiometry of ultra-thin films under 10 nm transforms from the Fe 3 O 4 phase to the FeO phase. In this work, a phase diagram based on thickness and oxygen pressure has been constructed to explain the structural phase transformation. It was found that high-quality magnetite films with thicknesses ≤20 nm formed within a narrow range of oxygen pressure. An optimal and controlled growth process is a crucial requirement for the accurate study of the magnetic and electronic properties for ultra-thin Fe 3 O 4 films. Furthermore, these results are significant because they may indicate a general trend in the growth of other oxide films, which has not been previously observed or considered.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Tunneling spectroscopy of c -axis epitaxial cuprate junctions

Atomically precise epitaxial structures are unique systems for tunneling spectroscopy that minimize extrinsic effects of disorder. We present a systematic tunneling spectroscopy study, over a broad doping, temperature, and bias range, in epitaxial c-axis La 2-x Sr x CuO 4 /La 2 CuO 4 /La 2-x Sr x CuO 4 heterostructures. The behavior of these superconductor/insulator/superconductor (SIS) devices is unusual. Down to 20 mK there is complete suppression of c-axis Josephson critical current with a barrier of only 2 nm of La 2 CuO 4 , and the zero-bias conductance remains at 20–30% of the normal-state conductance, implying a substantial population of in-gap states. Tunneling spectra show greatly suppressed coherence peaks. Furthermore, as the temperature is raised, the superconducting gap fills in rather than closing at T c . For all doping levels, the spectra show an inelastic tunneling feature at ~80 meV, suppressed as T exceeds T c . These nominally simple epitaxial cuprate junctions deviate markedly from expectations based on the standard Bardeen-Cooper-Schrieffer theory.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Manipulating the metal-to-insulator transition and magnetic properties in manganite thin films via epitaxial strain

Strain engineering of epitaxial transition metal oxide heterostructures offers an intriguing opportunity to control electronic structures by modifying the interplay between spin, charge, orbital, and lattice degrees of freedom. Here, we demonstrate that the electronic structure, magnetic and transport properties of La 0.9 Ba 0.1 MnO 3 thin films can be effectively controlled by epitaxial strain. Spectroscopic studies and first-principles calculations reveal that the orbital occupancy in Mn eg orbitals can be switched from the d 3z 2 -r 2 orbital to the d x 2 -y 2 orbital by varying the strain from compressive to tensile. Further, the change of orbital occupancy associated with Mn 3d-O 2p hybridization leads to dramatic modulation of the magnetic and electronic properties of strained La 0.9 Ba 0.1 MnO 3 thin films. Under moderate tensile strain, an emergent ferromagnetic insulating state with an enhanced ferromagnetic Curie temperature of 215 K is achieved. These findings not only deepen our understanding of electronic structures, magnetic and transport properties in the La 0.9 Ba 0.1 MnO 3 system, but also demonstrate the use of epitaxial strain as an effective knob to tune the electronic structures and related physical properties for potential spintronic device applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Strain tuning of electronic structure in Bi 4 Ti 3 O 12 -LaCoO 3 epitaxial thin films

In this study, we investigated the crystal and electronic structures of ferroelectric Bi 4 Ti 3 O 12 single-crystalline thin films site-specifically substituted with LaCoO 3 (LCO). The epitaxial films were grown by pulsed laser epitaxy on NdGaO 3 and SrTiO 3 substrates to vary the degree of strain. With increasing the LCO substitution, we observed a systematic increase in the c-axis lattice constant of the Aurivillius phase related with the modification of pseudo-orthorhombic unit cells. These compositional and structural changes resulted in a systematic decrease in the band gap, i.e., the optical transition energy between the oxygen 2p and transition-metal 3d states, based on a spectroscopic ellipsometry study. In particular, the Co 3d state seems to largely overlap with the Ti t 2g state, decreasing the band gap. Interestingly, the applied tensile strain facilitates the band-gap narrowing, demonstrating that epitaxial strain is a useful tool to tune the electronic structure of ferroelectric transition-metal oxides.

36 MATERIALS SCIENCE↗