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Generalized ellipsometry measurements are used to extract the complex dielectric function (ε = ε 1 + i ε 2) spectra of GdScO3 single crystals over the 0.7–8.5 eV photon energy range. GdScO3 is a wide bandgap semiconductor with a high dielectric constant, and potential applications include replacing SiO2 in silicon-based transistors and as an epitaxial substrate for thin film growth. This work presents the anisotropic optical properties for electric fields oscillating parallel to the a-, b-, and c-crystallographic axes. A direct bandgap is identified at 6.44 eV along the direction parallel to the a-axis, with additional critical points observed at 6.74 and 7.42 eV in the same direction. Additional above gap critical point transitions are found at 6.72, 7.31, and 7.96 along the direction parallel to the b-axis and 6.83 and 8.00 eV along the direction parallel to the c-axis. [ABSTRACT FROM AUTHOR]

We review recent developments and advances in the synthesis of thin-film multiferroic and magnetoelectric heterostructures. Driven by the promise of new materials with built-in useful phenomena (i.e., electric field control of ferromagnetism), extensive research has been centered on the search for and characterization of new single-phase multiferroic materials. In this review we provide a brief overview of recent developments in the synthesis of thin film versions of these materials. Advances in modern film growth processes have provided access to high-quality materials for in-depth study. We highlight the use of epitaxial thin-film strain to stabilize metastable phases, drive multiferroic properties, and produce new structures and properties in materials including case studies of EuTiO3 and BiFeO3. © 2012 Elsevier Ltd. All rights reserved.

Epitaxial untwinned SrRuO3 thin films were grown on (110)-oriented DyScO3 substrates by molecular-beam epitaxy. We report an exceptional sample with a residual resistivity ratio (RRR), ρ [300 K]/ρ [4 K] of 205 and a ferromagnetic Curie temperature, TC, of 168.3 K. We compare the properties of this sample to other SrRuO3 films grown on DyScO3(110) with RRRs ranging from 8.8 to 205, and also compare it to the best reported bulk single crystal of SrRuO3. We determine that SrRuO3 thin films grown on DyScO3(110) have an enhanced TC as long as the RRR of the thin film is above a minimum electrical quality threshold. This RRR threshold is about 20 for SrRuO3. Films with lower RRR exhibit TCs that are significantly depressed from the intrinsic strain-enhanced value. [ABSTRACT FROM AUTHOR]

TbScO3 is a wide bandgap semiconductor with potential applications in charge trap memory devices and acts as an alternate gate dielectric in fully depleted transistors and also a substrate for epitaxial thin film growth. TbScO3 has an orthorhombic crystal structure, which gives rise to optical anisotropy. Generalized ellipsometric spectra are measured for multiple in-plane rotations of (110) and (001) oriented TbScO3 single crystals over a photon energy range of 0.7–8.5 eV to determine the complex dielectric function (ε = ε1 + iε2) spectra for electric fields oscillating along each axis. A direct bandgap is identified at 6.50 eV, and above gap critical point transitions are found at 6.99, 7.14, 7.16, 7.21, and 7.42 eV. [ABSTRACT FROM AUTHOR]

New properties and exotic quantum phenomena can form due to periodic nanotextures, including Moire patterns, ferroic domains, and topologically protected magnetization and polarization textures. Despite the availability of powerful tools to characterize the atomic crystal structure, the visualization of nanoscale strain-modulated structural motifs remains challenging. Here, we develop nondestructive real-space imaging of periodic lattice distortions in thin epitaxial films and report an emergent periodic nanotexture in a Mott insulator. Specifically, we combine iterative phase retrieval with unsupervised machine learning to invert the diffuse scattering pattern from conventional X-ray reciprocal-space maps into real-space images of crystalline displacements. Our imaging in PbTiO3/SrTiO3 superlattices exhibiting checkerboard strain modulation substantiates published phase-field model calculations. Furthermore, the imaging of biaxially strained Mott insulator Ca2RuO4 reveals a strain-induced nanotexture comprised of nanometer-thin metallic-structure wires separated by nanometer-thin Mott-insulating-structure walls, as confirmed by cryogenic scanning transmission electron microscopy (cryo-STEM). The nanotexture in Ca2RuO4 film is induced by the metal-to-insulator transition and has not been reported in bulk crystals. We expect the phasing of diffuse X-ray scattering from thin crystalline films in combination with cryo-STEM to open a powerful avenue for discovering, visualizing, and quantifying the periodic strain-modulated structures in quantum materials. [ABSTRACT FROM AUTHOR]

Strain-engineering is a powerful means to tune the polar, structural, and electronic instabilities of incipient ferroelectrics. KTaO3 is near a polar instability and shows anisotropic superconductivity in electron-doped samples. Here, we demonstrate growth of high-quality KTaO3 thin films by molecular-beam epitaxy. Tantalum was provided by either a suboxide source emanating a TaO2 flux from Ta2O5 contained in a conventional effusion cell or an electron-beam-heated tantalum source. Excess potassium and a combination of ozone and oxygen (10% O3 + 90% O2) were simultaneously supplied with the TaO2 (or tantalum) molecular beams to grow the KTaO3 films. Laue fringes suggest that the films are smooth with an abrupt film/substrate interface. Cross-sectional scanning transmission electron microscopy does not show any extended defects and confirms that the films have an atomically abrupt interface with the substrate. Atomic force microscopy reveals atomic steps at the surface of the grown films. Reciprocal space mapping demonstrates that the films, when sufficiently thin, are coherently strained to the SrTiO3 (001) and GdScO3 (110) substrates. [ABSTRACT FROM AUTHOR]

Functional properties of transition-metal oxides strongly depend on crystallographic defects; crystallographic lattice deviations can affect ionic diffusion and adsorbate binding energies. Scanning x-ray nanodiffraction enables imaging of local structural distortions across an extended spatial region of thin samples. Yet, localized lattice distortions remain challenging to detect and localize using nanodiffraction, due to their weak diffuse scattering. Here, we apply an unsupervised machine learning clustering algorithm to isolate the low-intensity diffuse scattering in as-grown and alkaline-treated thin epitaxially strained SrIrO3 films. We pinpoint the defect locations, find additional strain variation in the morphology of electrochemically cycled SrIrO3, and interpret the defect type by analyzing the diffraction profile through clustering. Our findings demonstrate the use of a machine learning clustering algorithm for identifying and characterizing hard-to-find crystallographic defects in thin films of electrocatalysts and highlight the potential to study electrochemical reactions at defect sites in operando experiments. [ABSTRACT FROM AUTHOR]

Transport properties of electron-doped cuprate Sr 1 − x La x CuO 2 thin films have been investigated as a function of doping. In particular, optimal- and over-doped samples were obtained by tuning the Sr:La stoichiometric ratio. Optimal-doped samples show a non-Fermi liquid behavior characterized by linear dependence of the resistivity from room temperature down to intermediate temperature (about 150–170 K). However, by approaching temperatures in the superconducting transition, a Fermi-liquid behavior-characterized by a T 2 -scaling law-was observed. Once established, the transition from a linear-T to a quadratic- T 2 behavior was successfully traced back in over-doped samples, even occurring at lower temperatures. In addition, the over-doped samples show a crossover to a linear-T to a logarithmic dependence at high temperatures compatible with anti-ferromagnetic spin fluctuations dominating the normal state properties of electron-doped cuprates. [ABSTRACT FROM AUTHOR]

The unconventional superconductivity in Sr2RuO4 is infamously susceptible to suppression by small levels of disorder such that it has been most commonly studied in extremely high-purity bulk crystals. Here, we harness local structural and spectroscopic scanning transmission electron microscopy measurements in epitaxial thin films of Sr2RuO4 to disentangle the impact of different types of crystalline disorder on superconductivity. We find that cation off-stoichiometry during growth gives rise to two distinct types of disorder: mixed-phase structural inclusions that accommodate excess ruthenium and ruthenium vacancies when the growth is ruthenium-deficient. Several superconducting films host mixed-phase intergrowths, suggesting this microstructural disorder has relatively little impact on superconductivity. In a non-superconducting film, on the other hand, we measure a high density of ruthenium-vacancies (∼ 14 %) with no significant reduction in the crystallinity of the film. The results suggest that ruthenium vacancy disorder, which is hidden to many structural probes, plays an important role in suppressing superconductivity. We discuss the broader implications of our findings to guide the future synthesis of this and other layered systems. [ABSTRACT FROM AUTHOR]

Straining the vanadium dimers along the rutile c‐axis can be used to tune the metal‐to‐insulator transition (MIT) of VO2 but has thus far been limited to TiO2 substrates. In this work VO2/MgF2 epitaxial films are grown via molecular beam epitaxy (MBE) to strain engineer the transition temperature (TMIT). First, growth parameters are optimized by varying the synthesis temperature of the MgF2 (001) substrate (TS) using a combination of X‐ray diffraction techniques, temperature dependent transport, and soft X‐ray photoelectron spectroscopy. It is determined that TS values greater than 350 °C induce Mg and F interdiffusion and ultimately the relaxation of the VO2 layer. Using the optimized growth temperature, VO2/MgF2 (101) and (110) films are then synthesized. The three film orientations display MITs with transition temperatures in the range of 15–60 °C through precise strain engineering. [ABSTRACT FROM AUTHOR]

We have studied the growth of epitaxial films of stannate pyrochlores with a general formula A2Sn2O7 (A = La and Y) and find that it is possible to incorporate ∼25% excess of the A-site constituent; in contrast, any tin excess is expelled. We unravel the defect chemistry, allowing for the incorporation of excess A-site species and the mechanism behind the tin expulsion. An A-site surplus is manifested by a shift in the film diffraction peaks, and the expulsion of tin is apparent from the surface morphology of the film. In an attempt to increase La2Sn2O7 conductivity through n-type doping, substantial quantities of tin have been substituted by antimony while maintaining good film quality. The sample remained insulating as explained by first-principles computations, showing that both the oxygen vacancy and antimony-on-tin substitutional defects are deep. Similar conclusions are drawn on Y2Sn2O7. An alternative n-type dopant, fluorine on oxygen, is shallow according to computations and more likely to lead to electrical conductivity. The bandgaps of stoichiometric La2Sn2O7 and Y2Sn2O7 films were determined by spectroscopic ellipsometry to be 4.2 eV and 4.48 eV, respectively. [ABSTRACT FROM AUTHOR]

Using epitaxial stabilization, we synthesized single-phase (001)-oriented thin films of DyFe2O4+x on (111) MgAl2O4 substrates by molecular-beam epitaxy. The metastable DyFe2O4 polymorph formed is isostructural to known trigonal ferrimagnetic RFe2O4 phases with space group R 3 ̄ m , where R = Ho to Lu. The epitaxial DyFe2O4 thin films have two in-plane orientation relationships: [100] DyFe2O4 || 2 11 ̄ MgAl2O4 plus a twin variant related by a 60° in-plane rotation. DyFe2O4 is not bulk stable and has never been synthesized before. Indeed, it has been predicted to be on the edge energetically of what may be possible to stabilize. The fact that the RFe2O4 phase is stable for all elements leading up to dysprosium (Ho–Lu) leads us to believe that DyFe2O4 could be a "remnant metastable phase," one which, given the right thermodynamic conditions, could become the lowest free energy phase. We find that although we are able to get structurally very close to R 3 ̄ m DyFe2O4, the films are not stoichiometric as they have an increased c lattice parameter, indicative of extra oxygen as is sometimes seen in other RFe2O4 phases. The unintended surplus oxygen opens questions regarding what may be achievable using such tricks as epitaxial stabilization to access metastable phases and whether this indeed constitutes "remnant metastability." [ABSTRACT FROM AUTHOR]

Bandgap engineering is central to the design of heterojunction devices. For heterojunctions involving monolayer-thick materials like MoS2, the carrier concentration of the atomically thin film can vary significantly depending on the amount of charge transfer between MoS2 and the substrate. This makes substrates with a range of charge neutrality levels—as is the case for complex oxide substrates—a powerful addition to electrostatic gating or chemical doping to control the doping of overlying MoS2 layers. We demonstrate this approach by growing monolayer MoS2 on perovskite (SrTiO3 and LaAlO3), spinel (MgAl2O4), and SiO2 substrates with multi-inch uniformity. The as-grown MoS2 films on these substrates exhibit a controlled, reproducible, and uniform carrier concentration ranging from (1–4) ×1013 cm−2, depending on the oxide substrate employed. The observed carrier concentrations are further confirmed by our density-functional theory calculations based on ab initio mismatched interface theory (MINT). This approach is relevant to large-scale heterostructures involving monolayer-thick materials in which it is desired to precisely control carrier concentrations for applications. [ABSTRACT FROM AUTHOR]

Unlike many superlattice structures, Ruddlesden–Popper phases have atomically abrupt interfaces useful for interrogating how periodic atomic layers affect thermal properties. Here, we measure the thermal conductivity in thin films of the n = 1–5 and 10 members of the (SrTiO3)nSrO Ruddlesden–Popper superlattices grown by molecular-beam epitaxy and compare the results to a single crystal of the n = 1 Ruddlesden–Popper SrLaAlO4. The thermal conductivity cross-plane to the superlattice layering (k33) is measured using time-domain thermoreflectance as a function of temperature and the results are compared to first-principles calculations. The thermal conductivity of this homologous series decreases with increasing interface density. Characterization by x-ray diffraction and scanning transmission electron microscopy confirms that these samples have a Ruddlesden–Popper superlattice structure. [ABSTRACT FROM AUTHOR]

There has been significant progress on the fundamental science and technological applications of complex oxides and multiferroics. Among complex oxide thin films, barium strontium titanate (BST) has become the material of choice for room-temperature-based voltage-tunable dielectric thin films, due to its large dielectric tunability and low microwave loss at room temperature. BST thin film varactor technology based reconfigurable radio frequency (RF)/microwave components have been demonstrated with the potential to lower the size, weight, and power needs of a future generation of communication and radar systems. Low-power multiferroic devices have also been recently demonstrated. Strong magneto-electric coupling has also been demonstrated in different multiferroic heterostructures, which show giant voltage control of the ferromagnetic resonance frequency of more than two octaves. This manuscript reviews recent advances in the processing, and application development for the complex oxides and multiferroics, with the focus on voltage tunable RF/microwave components. The over-arching goal of this review is to provide a synopsis of the current state-of the-art of complex oxide and multiferroic thin film materials and devices, identify technical issues and technical challenges that need to be overcome for successful insertion of the technology for both military and commercial applications, and provide mitigation strategies to address these technical challenges. [ABSTRACT FROM AUTHOR]

We have measured the angle-resolved transverse resistivity (ARTR), a sensitive indicator of electronic anisotropy, in highquality thin films of the unconventional superconductor Sr2RuO4 grown on various substrates. The ARTR signal, heralding the electronic nematicity or a large nematic susceptibility, is present and substantial already at room temperature and grows by an order of magnitude upon cooling down to 4 K. In Sr2RuO4 films deposited on tetragonal substrates the highest-conductivity direction does not coincide with any crystallographic axis. In films deposited on orthorhombic substrates it tends to align with the shorter axis; however, the magnitude of the anisotropy stays the same despite the large lattice distortion. These are strong indications of actual or incipient electronic nematicity in Sr2RuO4. [ABSTRACT FROM AUTHOR]

This perspective considers the enormous promise of epitaxial functional transition metal oxide thin films for future applications in low power electronic and energy applications since they offer wide-ranging and highly tunable functionalities and multifunctionalities, unrivaled among other classes of materials. It also considers the great challenges that must be overcome for transition metal oxide thin films to meet what is needed in the application domain. These challenges arise from the presence of intrinsic defects and strain effects, which lead to extrinsic defects. Current conventional thin film deposition routes often cannot deliver the required perfection and performance. Since there is a strong link between the physical properties, defects and strain, routes to achieving more perfect materials need to be studied. Several emerging methods and modifications of current methods are presented and discussed. The reasons these methods better address the perfection challenge are considered and evaluated. [ABSTRACT FROM AUTHOR]

A major challenge for ferroelectric devices is the depolarization field, which competes with and often destroys long-range polar order in the limit of ultrathin films. Recent theoretical predictions suggest a new class of materials, termed hyperferroelectics, that should be robust against the depolarization field and enable ferroelectricity down to the monolayer limit. Here, the authors demonstrate the epitaxial growth of hexagonal LiZnSb, one of the hyperferroelectric candidate materials, by molecular-beam epitaxy on GaSb (111)B substrates. Due to the high volatility of all three atomic species, they find that LiZnSb can be grown in an adsorption-controlled window, using an excess zinc flux. Within this window, the desired polar hexagonal phase is stabilized with respect to a competing cubic polymorph, as revealed by x-ray diffraction and transmission electron microscopy measurements. First-principles calculations show that for moderate amounts of epitaxial strain and moderate concentrations of Li vacancies, the cubic LiZnSb phase is lower in formation energy than the hexagonal phase, but only by a few millielectronvolts per formula unit. Therefore, they suggest that kinetics plays a role in stabilizing the desired hexagonal phase at low temperatures. Their results provide a path toward experimentally demonstrating ferroelectricity and hyperferroelectricity in a new class of ternary intermetallic compounds. [ABSTRACT FROM AUTHOR]

Microwave tunable dielectric properties of strained (001) SrTiO3 thin films epitaxially deposited on (110) DyScO3 substrates were studied for in-plane film orientations ([100], [010], [110], and [-110]). A significant in-plane anisotropy in dielectric constant and tuning was observed in these SrTiO3 films. The highest dielectric constant and tuning at room temperature are observed along the [010] direction of the SrTiO3 film (1000 Å thick) (3500 and 70% at 1 V/μm, respectively), the lowest ones are observed along the [100] direction (i.e., 2000 and 50% at 1 V/μm, respectively). The dielectric constant and tuning along [-110] and [110] are about 2500 and 30% at 1 V/μm, respectively, which are intermediary to those along the [010] and [100] directions. The dielectric Q(=1/tan δ) does not show any large difference for the four directions (i.e., Q∼10-20). Also, the phase-transition peak for the [-110] and [110] directions of the SrTiO3 film (300 Å thick) is observed at 275 K, which is lower than that for the [010] and [100] directions. The observed in-plane anisotropic dielectric properties have been interpreted based on the phenomenological thermodynamics of film strain. [ABSTRACT FROM AUTHOR]

Structural distortion of ferroelectric thin films caused by film strain has a strong impact on the microwave dielectric properties. SrTiO3 thin films epitaxially grown on (110) DyScO3 substrates using molecular beam epitaxy are extremely strained (i.e., ∼1% in-plane tensional strain) from 3.905 Å of bulk SrTiO3. The room-temperature in-plane dielectric constant and its tuning of the films at 10 GHz are observed to be 6000 and 75% with an electric field of 1 V/μm, respectively. The control of strain in SrTiO3 provides a basis for room-temperature tunable microwave applications by elevating its phase-transition peak to room temperature. [ABSTRACT FROM AUTHOR]

Electric-field induced rearrangement of domain microstructure in an epitaxial thin film of Bi[sub 4]Ti[sub 3]O[sub 12] on a SrTiO[sub 3] (001) substrate is studied by optical second harmonic generation measurements. The input polarization dependence of the second harmonic signal exhibits spatial symmetries that reflect the presence of eight different domain variants present in the film. Changes in these symmetries with the application of electric field are experimentally studied at 23° C and 60 °C, and theoretically modeled to extract the hysteresis loops that reflect quantitative changes in the fraction of domain variants. A strong correlation is observed between the dc electrical conductance (as distinct from transient currents) and the ferroelectric domain state of the film, which is proposed to arise from the creation and destruction of charged domain walls within the film with applied field. © 2001 American Institute of Physics. [ABSTRACT FROM AUTHOR]

We report the in situ, direct epitaxial synthesis of (0001)-oriented PdCoO2 thin films on c-plane sapphire using ozone-assisted molecular-beam epitaxy. The resulting films have smoothness, structural perfection, and electrical characteristics that rival the best in situ grown PdCoO2 thin films in the literature. Metallic conductivity is observed in PdCoO2 films as thin as ∼2.0 nm. The PdCoO2 films contain 180° in-plane rotation twins. Scanning transmission electron microscopy reveals that the growth of PdCoO2 on the (0001) surface of Al2O3 begins with the CoO2 layer. [ABSTRACT FROM AUTHOR]

La-doped BaSnO3 has been epitaxially integrated with (001) Si using an SrTiO3 buffer layer via molecular-beam epitaxy (MBE). A 254 nm thick undoped BaSnO3 buffer layer was grown to enhance the mobility of the overlying La-doped BaSnO3 layer. The x-ray diffraction rocking curve of the BaSnO3 002 peak has a full width at half maximum of 0.02°. At room temperature, the resistivity of the La-doped BaSnO3 film is 3.6 × 10−4 Ω cm and the mobility is 128 cm2 V−1 s−1 at a carrier concentration of 1.4 × 1020 cm−3. These values compare favorably to those of La-doped BaSnO3 films grown by all techniques other than MBE on single-crystal oxide substrates. Our work opens an exciting arena for integrating hyper-functional oxide electronics that make use of high-mobility oxide films with the workhorse of the semiconductor industry, silicon. [ABSTRACT FROM AUTHOR]

We report the growth of superconducting Sr2RuO4 thin films by molecular-beam epitaxy on (110) NdGaO3 substrates with transition temperatures of up to 1.8 K. We calculate and experimentally validate a thermodynamic growth window for the adsorption-controlled growth of superconducting Sr2RuO4 epitaxial thin films. The growth window for achieving superconducting Sr2RuO4 thin films is narrow in growth temperature, oxidant pressure, and ruthenium-to-strontium flux ratio. [ABSTRACT FROM AUTHOR]

Abstract: Voltage‐tunable dielectric materials are widely used for microwave‐frequency signal processing. Among tunable dielectric thin films, (SrTiO3)nSrO Ruddlesden–Popper (RP) superlattices have exceptionally low loss at high frequencies. This paper reports the first realization of resonators, a ubiquitous building block of microwave components, fabricated on RP films, and an analysis of their static and dynamic tuning behavior. The RP film has a ferroelectric‐paraelectric phase transition at ≈200 K, and the tunability is strongest at this temperature. The resonators have approximately 2.5% tuning of the resonance frequency at room temperature and 20% tuning at 200 K, and a tuning time scale of less than a nanosecond, which is limited by the measurement circuit rather than material properties. [ABSTRACT FROM AUTHOR]

Epitaxial SrRuO3 and CaRuO3 films were grown under an excess flux of elemental ruthenium in an adsorption-controlled regime by molecular-beam epitaxy (MBE), where the excess volatile RuOx (x = 2 or 3) desorbs from the growth front leaving behind a single-phase film. By growing in this regime, we were able to achieve SrRuO3 and CaRuO3 films with residual resistivity ratios (ρ300 K/ρ4 K) of 76 and 75, respectively. A combined phase stability diagram based on the thermodynamics of MBE (TOMBE) growth, termed a TOMBE diagram, is employed to provide improved guidance for the growth of complex materials by MBE. [ABSTRACT FROM AUTHOR]

Generalized ellipsometry measurements are used to extract the complex dielectric function (ε = ε 1 + i ε 2) spectra of GdScO3 single crystals over the 0.7–8.5 eV photon energy range. GdScO3 is a wide bandgap semiconductor with a high dielectric constant, and potential applications include replacing SiO2 in silicon-based transistors and as an epitaxial substrate for thin film growth. This work presents the anisotropic optical properties for electric fields oscillating parallel to the a-, b-, and c-crystallographic axes. A direct bandgap is identified at 6.44 eV along the direction parallel to the a-axis, with additional critical points observed at 6.74 and 7.42 eV in the same direction. Additional above gap critical point transitions are found at 6.72, 7.31, and 7.96 along the direction parallel to the b-axis and 6.83 and 8.00 eV along the direction parallel to the c-axis. [ABSTRACT FROM AUTHOR]

A custom-built apparatus for performing rotating disk electrode voltammetry (RDE) using vapor-deposited, epitaxial, thin film samples as rotating electrodes is described. This method allows for quantitative electrochemical characterization using thin film samples, including those deposited on insulating substrates, and allows for very facile exchange of samples. Cyclic voltammetry and RDE voltammetry of iron ferricyanide in aqueous media were explored to examine if the system causes unusual deviations from ideal hydrodynamic voltammetric behavior. The set-up was also used to examine the ORR activity of a platinum thin film as a model system for a higher-current reaction, relevant to fuel-cell research. Both studies indicated that the set-up did not cause any deviations from anticipated RDE behavior, demonstrating that this is a viable method for performing rotating disk electrode voltammetry of vapor-deposited thin films, with emphasis on those relevant to fuel cell research. The set-up was used to investigate/test the ORR and OER activity of a series of A2B2O7 pyrochlore samples. [ABSTRACT FROM AUTHOR]

In numerous symmetric θ-2θ scans of phase-pure epitaxial complex oxide thin films grown on single-crystal substrates, we observe x-ray diffraction peaks that correspond to neither the film nor the substrate crystal structure. These peaks are the result of multiple, sequential diffraction events that occur from both the film and the substrate. The occurrence of so-called “hybrid” reflections, while described in the literature, is not widely reported within the complex oxide thin-film community. We describe a simple method to predict and identify peaks resulting from hybrid reflections and show examples from epitaxial complex oxide films belonging to three distinct structural types. [ABSTRACT FROM AUTHOR]

We demonstrate the ability to tune the thermal conductivity of homoepitaxial SrTiO3 films deposited by reactive molecular-beam epitaxy by varying growth temperature, oxidation environment, and cation stoichiometry. Both point defects and planar defects decrease the longitudinal thermal conductivity (k33), with the greatest decrease in films of the same composition observed for films containing planar defects oriented perpendicular to the direction of heat flow. The longitudinal thermal conductivity can be modified by as much as 80%--from 11.5W m-1K-1 for stoichiometric homoepitaxial SrTiO3 to 2W m-1K-1 for strontium-rich homoepitaxial Sr1þdTiOx films--by incorporating (SrO)2 Ruddlesden-Popper planar defects. [ABSTRACT FROM AUTHOR]

Superconductivity is a quantum state of matter characterized by the formation of Cooper pairs from time-reversal-symmetric electronic states. Mechanisms that break this symmetry, such as magnetic-impurity scattering and applied magnetic fields, are expected to be detrimental to superconductivity and suppress the critical temperature. Here, we report the observation of pronounced increases in the mean-field critical temperature on application of a parallel magnetic field in two different two-dimensional superconducting systems: ultrathin, homogeneously disordered amorphous Pb films and the two-dimensional electron gas at the interface of LaAlO3 and SrTiO3. In the amorphous Pb films, the critical-temperature increases exhibit a systematic dependence on the film thickness. Significantly, the presence of paramagnetic impurities in the films diminishes the effect of field enhancement of superconductivity. These observations mark a radical departure from the current understanding of the interactions between magnetic fields and superconductivity. [ABSTRACT FROM AUTHOR]

BiFeO3 thin films have been deposited on (001) SrTiO3, (101) DyScO3, (011) DyScO3, (0001) AlGaN/GaN, and (0001) 6H-SiC sungle crystal substrates by reactive molecular beam epitaxy in an absorption-controlled growth regime. This is achieved by supplying a bismuth over-pressure and utilizing the differential vapor pressures between bismuth oxides and BiFeO3 to control stoichiometry in accordance with thermodynamic calculations. Four-circle x-ray diffraction and transmission electron microscopy reveal phase-pure, epitaxial films with rocking curve full width at half maximum values as narrow as 7.2 arc seconds (0.002°). Epitaxial growth of (0001)-oriented BiFeO3 thin films on (0001) GaN, including AlGaN HEMT structures, and (0001) SiC has been realized using intervening epitaxial (111) SrTiO3 / (100) TiO2 buffer layers. The epitaxial BiFeO3 thin films have 2 in-plane orientations: [11¯20] BiFeO3 ∣∣ [11¯20] GaN (SiC) plus a twin variant related by a 180° in-plane rotation. This epitaxial integration of the ferroelectric with the highest known polarization, BiFeO3, with high bandgap semiconductors is an important step toward novel field-effect devices. [ABSTRACT FROM AUTHOR]

The broad spectrum of electronic and optical properties exhibited by oxides offers tremendous opportunities for microelectronic devices, especially when a combination of properties in a single device is desired. Here we describe the use of reactive molecular-beam epitaxy and pulsed-laser deposition to synthesize functional oxides, including ferroelectrics, ferromagnets, and materials that are both at the same time. Owing to the dependence of properties on direction, it is often optimal to grow functional oxides in particular directions to maximize their properties for a specific application. But these thin film techniques offer more than orientation control; customization of the film structure down to the atomic-layer level is possible. Numerous examples of the controlled epitaxial growth of oxides with perovskite and perovskite-related structures, including superlattices and metastable phases, are shown. In addition to integrating functional oxides with conventional semiconductors, standard semiconductor practices involving epitaxial strain, confined thickness, and modulation doping can also be applied to oxide thin films. Results of fundamental scientific importance as well as results revealing the tremendous potential of utilizing functional oxide thin films to create devices with enhanced performance are described. [ABSTRACT FROM AUTHOR]

Predictions and measurements of the effect of biaxial strain on the properties of epitaxial ferroelectric thin films and superlattices are reviewed. Results for single-layer ferroelectric films of biaxially strained SrTiO3, BaTiO3, and PbTiO3 as well as PbTiO3/SrTiO3 and BaTiO3/SrTiO3 superlattices are described. Theoretical approaches, including first principles, thermodynamic analysis, and phase-field models, are applied to these biaxially strained materials, the assumptions and limitations of each technique are explained, and the predictions are compared. Measurements of the effect of biaxial strain on the paraelectric-to-ferroelectric transition temperature (TC) are shown, demonstrating the ability of percent-level strains to shift TC by hundreds of degrees in agreement with the predictions that predated such experiments. Along the way, important experimental techniques for characterizing the properties of strained ferroelectric thin films and superlattices, as well as appropriate substrates on which to grow them, are mentioned. [ABSTRACT FROM AUTHOR]

We have grown Bi2Sr2Co2Oy thin films on LaAlO3 (100) and fused silica substrates by pulsed laser deposition. The films on LaAlO3 are c-axis oriented and partially in-plane aligned with multiple domains, while the films on fused silica are preferred c-axis oriented without in-plane alignment. The Seebeck coefficient and resistivity of films on both substrates are comparable to those of single crystals. An oxide p-n heterojunction was formed by depositing Bi2Sr2Co2Oy film on Nb-doped SrTiO3 single crystal, which showed a rectifying behavior. These thin films and heterostructures may be used for future thermoelectric applications. [ABSTRACT FROM AUTHOR]

The structure of the SrTiO3/Si interface is determined by high-angle annular dark field imaging in combination with a recently developed technique based on aberration-corrected high-resolution transmission electron microscopy. At the interface, a monolayer of SrO faces the terminating plane of silicon. In this monolayer, the strontium atoms lie above the face-center of four silicon atoms in the terminating plane, and the oxygen atoms are located directly above the terminating silicon atoms. This structure, which is the dominant type of interface structure observed in this system, agrees with one of the interface structures predicted by first-principles calculations. [ABSTRACT FROM AUTHOR]

Commensurately strained epitaxial SrTiO3 thin films on a GdScO3 substrate with anisotropic in-plane tensile strains of 1.46% and 1.59% were grown. By using optical second harmonic generation and polarization measurements, a ferroelectric transition from a tetragonal 4/mmm phase to a ferroelectric mm2 phase at ∼400 K and an antiferrodistortive transition to a multiferroic phase at 150–175 K are observed, which are in agreement with thermodynamic calculations. In addition, a series of polarization rotation transitions between <100>p to p (0

Local frequency-dependent polar dynamics of strained SrTiO3 films grown on DyScO3 are investigated using time-resolved confocal scanning optical microscopy. Spectroscopic information is obtained with <1 μm spatial resolution over the frequency range 2–4 GHz. Most of the DyScO3 film is found to be spatially homogeneous, in contrast to relaxed films. A strong correlation between spatial and spectral homogeneity is revealed. In addition, resonant structures are discovered that are localized both in space and in frequency. [ABSTRACT FROM AUTHOR]

Large third-order optical nonlinearities were observed in epitaxial thin films of BiMnO[sub 3] grown on SrTiO[sub 3] substrates. Using 140 fs laser pulses at 900 nm, a negative nonlinear refractive index (n[sub I]∼-0.53 cm[sup 2]/GW) and a nonlinear absorption coefficient (α[sub I]∼-0.08 cm/kW) for BiMnO[sub 3] are measured at room temperature. Large electric-field-induced enhancement of three to four orders of magnitude in the second-harmonic response at 450 nm is observed with effective nonlinear coefficients of d[sub eff]∼40(115) pm/V at 300 (473) K under applied fields of ∼707 (177) V/mm, respectively, from a 110 nm multivariant thin film. © 2003 American Institute of Physics. [ABSTRACT FROM AUTHOR]

Reveals that an error has been made in the article 'Probing Domain Microstructure in Ferroelectric Bi[sub 4]Ti[sub 3]O[sub 12] Thin Films by Optical Second Harmonic Generation'. Incorrect ratios of nonlinear optical coefficients of Bi[sub 4]Ti[sub 3]O[sub 12] thin films; Minor typographical error in equation 7.

(001)-oriented LaAlO3 films were grown epitaxially on (001) Si substrates utilizing an ultrathin 5 unit-cell-thick SrTiO3 buffer layer. The SrTiO3 layer was grown at ∼250 °C and annealed in vacuum at 550 °C, following an epitaxy-by-periodic-annealing procedure. Upon this buffer layer, the LaAlO3 layer was then grown by codeposition at 580 °C. The rocking curve of the as-grown LaAlO3 film exhibits a full width at half maximum value as small as 0.02°. Atomic force microscopy shows that the surface of the LaAlO3 film has a root-mean-square roughness of 1.3 Å. Scanning transmission electron microscopy reveals that the LaAlO3/SrTiO3 interface and the SrTiO3/Si interfaces are sharp. This high crystalline quality, twin-free, epitaxial LaAlO3 on SrTiO3 on silicon could be relevant to integrating oxides with multiple functionalities on silicon. [ABSTRACT FROM AUTHOR]

TbScO3 is a wide bandgap semiconductor with potential applications in charge trap memory devices and acts as an alternate gate dielectric in fully depleted transistors and also a substrate for epitaxial thin film growth. TbScO3 has an orthorhombic crystal structure, which gives rise to optical anisotropy. Generalized ellipsometric spectra are measured for multiple in-plane rotations of (110) and (001) oriented TbScO3 single crystals over a photon energy range of 0.7–8.5 eV to determine the complex dielectric function (ε = ε1 + iε2) spectra for electric fields oscillating along each axis. A direct bandgap is identified at 6.50 eV, and above gap critical point transitions are found at 6.99, 7.14, 7.16, 7.21, and 7.42 eV. [ABSTRACT FROM AUTHOR]

We have measured the angle-resolved transverse resistivity (ARTR), a sensitive indicator of electronic anisotropy, in highquality thin films of the unconventional superconductor Sr2RuO4 grown on various substrates. The ARTR signal, heralding the electronic nematicity or a large nematic susceptibility, is present and substantial already at room temperature and grows by an order of magnitude upon cooling down to 4 K. In Sr2RuO4 films deposited on tetragonal substrates the highest-conductivity direction does not coincide with any crystallographic axis. In films deposited on orthorhombic substrates it tends to align with the shorter axis; however, the magnitude of the anisotropy stays the same despite the large lattice distortion. These are strong indications of actual or incipient electronic nematicity in Sr2RuO4. [ABSTRACT FROM AUTHOR]

A strain-driven orthorhombic (O) to rhombohedral (R) phase transition is reported in La-doped BiFeO3 thin films on silicon substrates. Biaxial compressive epitaxial strain is found to stabilize the rhombohedral phase at La concentrations beyond the morphotropic phase boundary (MPB). By tailoring the residual strain with film thickness, we demonstrate a mixed O/R phase structure consisting of O phase domains measuring tens of nanometers wide within a predominant R phase matrix. A combination of piezoresponse force microscopy (PFM), transmission electron microscopy (TEM), polarization-electric field hysteresis loop (P-E loop), and polarization maps reveal that the O-R structural change is an antiferroelectric to ferroelectric (AFE-FE) phase transition. Using scanning transmission electron microscopy (STEM), an atomically sharp O/R MPB is observed. Moreover, X-ray absorption spectra (XAS) and X-ray linear dichroism (XLD) measurements reveal a change in the antiferromagnetic axis orientation from out of plane (R-phase) to in plane (O-phase). These findings provide direct evidence of spin-charge-lattice coupling in La-doped BiFeO3 thin films. Furthermore, this study opens a new pathway to drive the AFE-FE O-R phase transition and provides a route to study the O/R MPB in these films. [ABSTRACT FROM AUTHOR]

The bronze polymorph of titanium dioxide, known as TiO2(B), has promising photochemical and electronic properties for potential applications in Li-ion batteries, photocatalysis, chemical sensing, and solar cells. In contrast to previous studies performed with powder samples, which often suffer from impurities and lattice water, here we report Raman spectra from highly crystalline TiO2(B) films epitaxially grown on Si substrates with a thin SrTiO3 buffer layer. The reduced background from the Si substrate significantly benefits acquisition of polarization-dependent Raman spectra collected from the high-quality thin films, which are compared to nanopowder results reported in the literature. The experimental spectra were compared with density functional theory calculations to analyze the atomic displacements associated with each Raman-active vibrational mode. These results provide a standard reference for further investigation of the crystallinity, structure, composition, and properties of TiO2(B) materials with Raman spectroscopy. [ABSTRACT FROM AUTHOR]

We locally investigate the electronictransport through individualtunnel junctions containing a 10 nm thin film of vanadium dioxide(VO2) across its thermally induced phase transition. Theinsulator-to-metal phase transition in the VO2film collapsesthe Hubbard gap (experimentally determined to be 0.4 ± 0.07 V),leading to several orders of magnitude change in tunnel conductance.We quantitatively evaluate underlying transport mechanisms via theoreticalquantum mechanical transport calculations which show excellent agreementwith the experimental results. [ABSTRACT FROM AUTHOR]

[Display omitted] • Successful integration of oxides (SrTiO 3 , La 2/3 Sr 1/3 MnO 3) on industrial compatible SOS wafers. • Successful fabrication of LSMO double clamped MEMS structures by silicon micromachining. • 3D topography of MEMS micro-bridge structures visualized by digital holographic microscopy. We report the integration of high-quality epitaxial La 2/3 Sr 1/3 MnO 3 (LSMO) thin films onto SrTiO 3 buffered Silicon-on-Sapphire (SOS) substrates by combining state-of-the-art thin film growth techniques such as molecular beam epitaxy and pulsed laser deposition. Detailed structural, magnetic and electrical characterizations of the LSMO/STO/SOS heterostructures show that the LSMO film properties are competitive with those directly grown on oxide substrates. X-ray magnetic circular dichroism measurements on Mn L 2,3 edges show strong dichroic signal at room temperature, and angular-dependent in-plane magnetic properties by magneto-optical Kerr magnetometry reveal isotropic magnetic anisotropy. Suspended micro-bridges were thus finally fabricated by silicon micromachining, thus demonstrating the potential use of integrating LSMO magnetic layer on industrially compatible SOS substrates for the development of applicative MEMS devices. [ABSTRACT FROM AUTHOR]