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Binary rutile oxides of 5d metals such as IrO2, stand out as a paradox due to limited experimental studies despite the rich predicted quantum phenomena. Here, we investigate the electrical transport properties of IrO2 by engineering epitaxial thin films grown via hybrid molecular beam epitaxy. Our findings reveal phonon-limited carrier transport and thickness-dependent anisotropic in-plane resistance in IrO2 (110) films, the latter suggesting a complex relationship between strain relaxation and orbital hybridization. Magneto-transport measurements reveal a previously unobserved non-linear Hall effect. A two-carrier analysis of this effect shows the presence of minority carriers with mobility exceeding 3000 cm2/Vs at 1.8 K. These results point towards emergent properties in 5d metal oxides that can be controlled using dimensionality and epitaxial strain., Comment: 16 pages

Water-soluble sacrificial layers based on epitaxially-grown, single crystalline (Ca, Sr, Ba)3Al2O6 layer are widely used for creating free-standing perovskite oxide membranes. However, obtaining these sacrificial layers with intricate stoichiometry remains a challenge, especially for molecular beam epitaxy (MBE). In this study, we demonstrate the hybrid MBE growth of epitaxial, single crystalline SrTiO3 films using a solution processed, amorphous SrCa2Al2O6 sacrificial layer onto SrTiO3 (001) substrates. Prior to the growth, the oxygen plasma exposure was used to first create the crystalline SrCa2Al2O6 layer with well-defined surface crystallinity. Utilizing reflection high energy electron diffraction, x-ray diffraction, and atomic force microscopy, we observe an atomic layer-by-layer growth of epitaxial, single crystalline SrTiO3 film on the SrCa2Al2O6 layer with atomically smooth surfaces. The SrCa2Al2O6 layer was subsequently dissolved in de-ionized water to create free-standing SrTiO3 membranes that were transferred onto a metal-coated Si wafer. Membranes created with Sr-deficiency revealed ferroelectric-like behavior measured using piezo force microscopy whereas stoichiometric films remained paraelectric-like. These findings underscore the viability of using ex-situ deposited amorphous SrCa2Al2O6 for epitaxial, single crystalline growth, as well as the importance of point defects in determining the ferroic properties in membranes., Comment: 16 pages

Exploration and advancements in ultra-wide bandgap (UWBG) semiconductors are pivotal for next-generation high-power electronics and deep-ultraviolet (DUV) optoelectronics. A critical challenge lies in finding a semiconductor that is highly transparent to DUV wavelengths yet conductive with high mobility at room temperature. Here, we achieved both high transparency and high conductivity by employing a thin heterostructure design. The heterostructure facilitated high conductivity by screening phonons using free carriers, while the atomically thin films ensured high transparency. We utilized a heterostructure comprising SrSnO3/La:SrSnO3/GdScO3 (110) and applied electrostatic gating to effectively separate electrons from their dopant atoms. This led to a modulation of carrier density from 1018 cm-3 to 1020 cm-3, with room temperature mobilities ranging from 40 to 140 cm2V-1s-1. The phonon-limited mobility, calculated from first principles, closely matched experimental results, suggesting that room-temperature mobility could be further increased with higher electron density. Additionally, the sample exhibited 85% optical transparency at a 300 nm wavelength. These findings highlight the potential of heterostructure design for transparent UWBG semiconductor applications, especially in deep-ultraviolet regime., Comment: 32 pages

Advances in material fabrication techniques and growth methods have opened up a new chapter for twistronics, in the form of twisted freestanding three-dimensional material membranes. Through first-principles calculations based on density functional theory, we investigate the crystal and electronic structures of twisted bilayer BaTiO$_3$. Our findings reveal that large stacking fault energy leads to chiral in-plane vortex pattern that was recently observed in experiments. Moreover, we also found non-zero out-of-plane local dipole moments, indicating that the strong interlayer interaction might offer promising strategy to stabilize ferroelectric order in the two-dimensional limit. Remarkably, the vortex pattern in the twisted BaTiO$_3$ bilayer support localized electronic states with quasi-flat bands, associated with the interlayer hybridization of oxygen $p_z$ orbitals. We found that the associated band width reaches a minimum at $\sim$19$^{\circ}$ twisting, configuring the largest magic angle in moir\'e systems reported so far. Further, the moir\'e vortex pattern bears a striking resemblance to two interpenetrating Lieb lattices and corresponding tight-binding model provides a comprehensive description of the evolution the moir\'e bands with twist angle and reveals the topological nature of these states., Comment: 8 pages, 5 figures

Altermagnetism refers to a wide class of compensated magnetic orders featuring magnetic sublattices with opposite spins related by rotational symmetry rather than inversion or translational operations, resulting in non-trivial spin splitting and high-order multipolar orders. Here, by combining theoretical analysis, electrical transport, X-ray and optical spectroscopies, and nonlinear optical measurements, we establish a phase diagram in hybrid molecular beam epitaxy-grown RuO2/TiO2 (110) films, mapping the broken symmetries along the altermagnetic/electronic/structural phase transitions as functions of film thickness and temperature. This phase diagram features a novel altermagnetic metallic polar phase in strained 2 nm samples, extending the concept of multiferroics to altermagnetic systems. These results provide a comprehensive understanding of altermagnetism upon epitaxial heterostructure design for emergent novel phases with multifunctionalities., Comment: 15 pages

The mechanism of superconductivity in materials with aborted ferroelectricity and the emergence of a dilute metallic phase in systems like doped-SrTiO$_3$ are outstanding issues in condensed matter physics. This dilute metal has features both similar and different to those found in the normal state of other unconventional superconductors. We have investigated the optical properties of the dilute metallic phase in doped-SrTiO$_3$ using THz time-domain spectroscopy. At low frequencies the THz response exhibits a Drude-like form as expected for typical metal-like conductivity. We observed the frequency and temperature dependencies to the low energy scattering rate $\Gamma(\omega, T) \propto (\hbar\omega)^2 + (p \pi k_BT)^2 $ expected in a conventional Fermi liquid, despite the fact that densities are too small to allow current decay through electron-electron scattering. However we find the lowest known $p$ values of 0.39-0.72. As $p$ is 2 in a canonical Fermi liquid and existing models based on energy dependent elastic scattering bound $p$ from below to 1, our observation lies outside current explanation. Our data also gives insight into the high temperature regime and shows that the temperature dependence of the resistivity derives in part from strong T dependent mass renormalizations., Comment: 6 pages, 4figures

Plan-view transmission electron microscopy (TEM) samples are key to understand the atomic structure and associated properties of materials along their growth orientation, especially for thin films that are stain-engineered onto different substrates for property tuning. In this work, we present a method to prepare high-quality plan-view samples for analytical STEM study from thin-films using a dual-beam focused ion beam scanning electron microscope (FIB-SEM) system. The samples were prepared from thin films of perovskite oxides and metal oxides ranging from 20-80 nm thicknesses, grown on different substrates using molecular beam epitaxy. A site-specific sample preparation from the area of interest is described, which includes sample attachment and thinning techniques to minimize damage to the final TEM samples. While optimized for the thin film-like geometry, this method can be extended to other site-specific plan-view samples from bulk materials. Aberration-corrected scanning (S)TEM was used to access the quality of the thin film in each sample. This enabled direct visualization of line defects in perovskite BaSnO3 and Ir particle formation and texturing in IrO2 films.

Epitaxially grown RuO2 films on TiO2 (110) exhibit significant in-plane strain anisotropy, with a compressive strain of - 4.7% along the [001] crystalline direction and a tensile strain of +2.3% along [1-10]. As the film thickness increases, anisotropic strain relaxation is expected. By fabricating Hall bar devices with current channels along two in-plane directions <001> and <1-10>, we revealed anisotropic in-plane transport in RuO2/TiO2 (110) films grown via solid-source metal-organic molecular beam epitaxy approach. For film thicknesses (t_film) < 3.6 nm, the resistivity along <001> exceeds that along <1-10> direction at all temperatures. With further decrease in film thicknesses, we uncover a transition from metallic to insulating behavior at t_film <2.1 nm. Our combined temperature- and magnetic field-dependent electrical transport measurements reveal that this transition from metallic to insulating behavior is driven by electron-electron interactions., Comment: 15 pages

The advancement in thin-film exfoliation for synthesizing oxide membranes has opened up new possibilities for creating artificially-assembled heterostructures with structurally and chemically incompatible materials. The sacrificial layer method is a promising approach to exfoliate as-grown films from a compatible material system, allowing their integration with dissimilar materials. Nonetheless, the conventional sacrificial layers often possess intricate stoichiometry, thereby constraining their practicality and adaptability, particularly when considering techniques like Molecular Beam Epitaxy (MBE). This is where easy-to-grow binary alkaline earth metal oxides with a rock salt crystal structure are useful. These oxides, which include (Mg, Ca, Sr, Ba)O, can be used as a sacrificial layer covering a much broader range of lattice parameters compared to conventional sacrificial layers and are easily dissolvable in deionized water. In this study, we show the epitaxial growth of single-crystalline perovskite SrTiO3 (STO) on sacrificial layers consisting of crystalline SrO, BaO, and Ba1-xCaxO films, employing a hybrid MBE method. Our results highlight the rapid (< 5 minutes) dissolution of the sacrificial layer when immersed in deionized water, facilitating the fabrication of millimeter-sized STO membranes. Using high-resolution x-ray diffraction, atomic-force microscopy, scanning transmission electron microscopy, impedance spectroscopy, and scattering-type near-field optical microscopy (SNOM), we demonstrate epitaxial STO membranes with bulk-like intrinsic dielectric properties. The employment of alkaline earth metal oxides as sacrificial layers is likely to simplify membrane synthesis, particularly with MBE, thus expanding research possibilities., Comment: 36 pages, 4 figures

We examine the effects of Pt vacancies on the magnetotransport properties of Weyl semimetal candidate GdPtSb films, grown by molecular beam epitaxy on c-plane sapphire. Rutherford backscattering spectrometry (RBS) and x-ray diffraction measurements suggest that phase pure GdPt$_{x}$Sb films can accommodate up to $15\%$ Pt vacancies ($x=0.85$), which act as acceptors as measured by Hall effect. Two classes of electrical transport behavior are observed. Pt-deficient films display a metallic temperature dependent resistivity (d$\rho$/dT$>$0). The longitudinal magnetoresistance (LMR, magnetic field $\mathbf{B}$ parallel to electric field $\mathbf{E}$) is more negative than transverse magnetoresistance (TMR, $\mathbf{B} \perp \mathbf{E}$), consistent with the expected chiral anomaly for a Weyl semimetal. The combination of Pt-vacancy disorder and doping away from the expected Weyl nodes; however, suggests conductivity fluctuations may explain the negative LMR rather than chiral anomaly. Samples closer to stoichiometry display the opposite behavior: semiconductor-like resistivity (d$\rho$/dT$<$0) and more negative transverse magnetoresistance than longitudinal magnetoresistance. Hysteresis and other nonlinearities in the low field Hall effect and magnetoresistance suggest that spin disorder scattering, and possible topological Hall effect, may dominate the near stoichiometric samples. Our findings highlight the complications of transport-based identification of Weyl nodes, but point to possible topological spin textures in GdPtSb.

Restructuring of rutile TiO$_{2}$ under electron beam irradiation driven by radiolysis was observed and analyzed using a combination of atomic-resolution imaging and electron energy loss spectroscopy (EELS) in scanning transmission electron microscopy (STEM). It was determined that a high-energy (80-300 keV) electron beam at high doses ($\gtrapprox 10^7 \ e/nm^2$) can constructively restructure rutile TiO$_{2}$ with an efficiency of $6\times 10^{-6}$. These observations were realized using rutile TiO$_{2}$ samples with atomically sharp nanometer-wide cracks. Based on atomic-resolution STEM imaging and quantitative EELS analysis, we propose a $"$ 2-step $"$ rolling model of the octahedral building blocks of the crystal to account for observed radiolysis-driven atomic migration., Comment: 15 pages with 5 figures

The epitaxial growth of functional materials using a substrate with a graphene layer is a highly desirable method for improving structural quality and obtaining free-standing epitaxial nano-membranes for scientific study, applications, and economical reuse of substrates. However, the aggressive oxidizing conditions typically employed to grow epitaxial perovskite oxides can damage graphene. Here, we demonstrate a technique based on hybrid molecular beam epitaxy that does not require an independent oxygen source to achieve epitaxial growth of complex oxides without damaging the underlying graphene. The technique produces films with self-regulating cation stoichiometry control and epitaxial orientation to the oxide substrate. Furthermore, the films can be exfoliated and transferred to foreign substrates while leaving the graphene on the original substrate. These results open the door to future studies of previously unattainable free-standing nano-membranes grown in an adsorption-controlled manner by hybrid molecular beam epitaxy, and has potentially important implications for the commercial application of perovskite oxides in flexible electronics., Comment: 20 pages, 6 figures

Germanium-based oxides such as rutile GeO2 are garnering attention owing to their wide band gaps and the prospects for ambipolar doping for application in high-power devices. Here, we present the use of germanium tetraisopropoxide (GTIP) (an organometallic chemical precursor) as a source of Ge for the demonstration of hybrid molecular beam epitaxy (MBE) for Ge-containing compounds. We use Sn1-xGexO2 and SrSn1-xGexO3 as model systems to demonstrate this new synthesis method. A combination of high-resolution X-ray diffraction, scanning transmission electron microscopy, and X-ray photoelectron spectroscopy confirms the successful growth of epitaxial rutile Sn1-xGexO2 on TiO2(001) substrates up to x = 0.54 and coherent perovskite SrSn1-xGexO3 on GdScO3(110) substrates up to x = 0.16. Characterization and first-principles calculations corroborate that Ge preferentially occupies the Sn site, as opposed to the Sr site. These findings confirm the viability of the GTIP precursor for the growth of germanium-containing oxides by hybrid MBE, and thus open the door to high-quality perovskite germanate films.

The study of subtle effects on transport in semiconductors requires high-quality epitaxial structures with low defect density. Using hybrid molecular beam epitaxy (MBE), SrTiO$_3$ films with low-temperature mobility exceeding 42,000 cm$^2$V$^{-1}$s$^{-1}$ at low carrier density of 3 x 10$^{17}$ cm$^{-3}$ were achieved. A sudden and sharp decrease in residual resistivity accompanied by an enhancement in the superconducting transition temperature were observed across the second Lifshitz transition (LT) where the third band becomes occupied, revealing dominant intra-band scattering. These films further revealed an anomalous behavior in the Hall carrier density as a consequence of the antiferrodistortive (AFD) transition and the temperature-dependence of the Hall scattering factor. Using hybrid MBE growth, phenomenological modeling, temperature-dependent transport measurements, and scanning superconducting quantum interference device imaging, we provide critical insights into the important role of inter- vs intra-band scattering and of AFD domain walls on normal-state and superconducting properties of SrTiO$_3$., Comment: 18 pages, 4 figures

Hysteretic magnetoresistance (MR) is often used as a signature of ferromagnetism in conducting oxide thin films and heterostructures. Here, magnetotransport is investigated in a non-magnetic uniformly La-doped SrSnO3 film grown using hybrid molecular beam epitaxy. A 12 nm La:SrSnO3/2 nm SrSnO3/GdScO3 (110) film with insulating behavior exhibited a robust hysteresis loop in the MR at T < 5 K accompanied by an anomaly at ~ +/- 3 T at T < 2.5 K. Furthermore, MR with the field in-plane yielded a value exceeded 100% at 1.8 K. Using detailed temperature-, angle- and magnetic field-dependent resistance measurements, we illustrate the origin of hysteresis is not due to magnetism in the film but rather is associated with the magnetocaloric effect of the GdScO3 substrate. Given GdScO3 and similar substrates are commonly used in complex oxide research, this work highlights the importance of thermal coupling to processes in the substrates which must be carefully accounted for in the data interpretation for thin films and heterostructures utilizing these substrates.

A seemingly simple oxide with a rutile structure, RuO2 has been shown to possess several intriguing properties ranging from strain-stabilized superconductivity to a strong catalytic activity. Much interest has arisen surrounding the controlled synthesis of RuO2 films but, unfortunately, utilizing atomically-controlled deposition techniques like molecular beam epitaxy (MBE) has been difficult due to the ultra-low vapor pressure and low oxidation potential of Ru. Here, we demonstrate the growth of epitaxial, single-crystalline RuO2 films on different substrate orientations using the novel solid-source metal-organic (MO) MBE. This approach circumvents these issues by supplying Ru using a pre-oxidized solid metal-organic precursor containing Ru. High-quality epitaxial RuO2 films with bulk-like room-temperature resistivity of 55 micro-ohm-cm were obtained at a substrate temperature as low as 300 C. By combining X-ray diffraction, transmission electron microscopy, and electrical measurements, we discuss the effect of substrate temperature, orientation, film thickness, and strain on the structure and electrical properties of these films. Our results illustrating the use of novel solid-source MOMBE approach paves the way to the atomic-layer controlled synthesis of complex oxides of stubborn metals, which are not only difficult to evaporate but also hard to oxidize., Comment: 21 pages including 6 figures

Distinct dopant behaviors inside and outside dislocation cores are identified by atomic-resolution electron microscopy in perovskite BaSnO3 with considerable consequences on local atomic and electronic structures. Driven by elastic strain, when A-site designated La dopants segregate near a dislocation core, the dopant atoms accumulate at the Ba sites in compressively strained regions. This triggers formation of Ba-vacancies adjacent to the core atomic sites resulting in reconstruction of the core. Notwithstanding the presence of extremely large tensile strain fields, when La atoms segregate inside the dislocation core, they become B-site dopants, replacing Sn atoms and compensating the positive charge of the core oxygen vacancies. Electron energy-loss spectroscopy shows that the local electronic structure of these dislocations changes dramatically due to the segregation of the dopants inside and around the core ranging from formation of strong La-O hybridized electronic states near the conduction band minimum to insulator-to-metal transition.

Perovskite alkaline earth stannates, such as $BaSnO_3$ and $SrSnO_3$, showing light transparency and high electrical conductivity (when doped), have become promising candidates for novel optoelectrical devices. Such devices are mostly based on hetero-structures and understanding of their electronic structure, which usually deviates from the bulk, is mandatory for exploring a full application potential. Employing angle-resolved photoemission spectroscopy and ab initio calculations we reveal the existence of a 2-dimensional metallic state at the $SnO_2$-terminated surface of a 1\% La-doped $BaSnO_3$ thin film. The observed surface state is characterized by distinct carrier density and a smaller effective mass in comparison with the corresponding bulk values. The small surface effective mass of about $0.12m_e$ can cause an improvement of the electrical conductivity of BSO based heterostructures.

SrSnO3 (SSO) is an emerging ultra-wide bandgap (UWBG) semiconductor with potential for highpower applications. In-plane compressive strain was recently shown to stabilize the high temperature tetragonal phase of SSO at room temperature (RT) which exists at T > 1062 K in bulk. Here, we report on the study of strain relaxation in epitaxial, tetragonal phase of Nd-doped SSO films grown on GdScO3 (110) (GSO) substrates using radical-based hybrid molecular beam epitaxy. The thinnest SSO film (thickness, t = 12 nm) yielded a fully coherent tetragonal phase at RT. At 12 nm < t < 110 nm, the tetragonal phase first transformed into orthorhombic phase and then at t > 110 nm, the orthorhombic phase began to relax by forming misfit dislocations. Remarkably, the tetragonal phase remained fully coherent until it completely transformed into the orthorhombic phase. Using thickness- and temperature-dependent electronic transport measurements, we discuss the important roles of the surface, phase coexistence, and misfit dislocations on carrier density and mobility in Nd-doped SSO. This study provides unprecedented insights into the strain relaxation behavior and its consequences for electronic transport in doped SSO with implications in the development of high-power electronic devices., Comment: 19 pages, 4 figures

By combining temperature-dependent resistivity and Hall effect measurements, we investigate donor state energy in Si-doped \b{eta}-Ga2O3 films grown using metal-organic vapor phase epitaxy (MOVPE). High magnetic field Hall effect measurements (H = +/-90 kOe) showed non-linear Hall resistance for T < 150 K revealing two-band conduction. Further analyses revealed carrier freeze-out characteristics in both bands yielding donor state energies of ~ 33.7 and ~ 45.6 meV. The former is consistent with the donor energy of Si in \b{eta}-Ga2O3 whereas the latter suggests a residual donor state, likely associated with a DX center. This study provides a critical insight into the impurity band conduction and the defect energy states in \b{eta}-Ga2O3 using high-field magnetotransport measurements., Comment: 14 pages

We describe a novel approach for the rational design and synthesis of self-assembled periodic nanostructures using martensitic phase transformations. We demonstrate this approach in a thin film of perovskite SrSnO3 with reconfigurable periodic nanostructures consisting of regularly spaced regions of sharply contrasted dielectric properties. The films can be designed to have different periodicities and relative phase fractions via chemical doping or strain engineering. The dielectric contrast within a single film can be tuned using temperature and laser wavelength, effectively creating a variable photonic crystal. Our results show the realistic possibility of designing large-area self-assembled periodic structures using martensitic phase transformations with the potential of implementing "built-to-order" nanostructures for tailored optoelectronic functionalities., Comment: 13 pages, 5 figures

As a prototypical Mott insulator with ferromagnetic ordering, YTiO3 (YTO) is of great interest in the study of strong electron correlation effects and orbital ordering. Here we report the first molecular beam epitaxy (MBE) growth of YTO films, combined with theoretical and experimental characterization of the electronic structure and charge transport properties. The obstacles of YTO MBE growth are discussed and potential routes to overcome them are proposed. DC transport and Seebeck measurements on thin films and bulk single crystals identify p-type Arrhenius transport behavior, with an activation energy of ~ 0.17 eV in thin films, consistent with the energy barrier for small hole polaron migration from hybrid density functional theory (DFT) calculations. Hard X-ray photoelectron spectroscopy measurements (HAXPES) show the lower Hubbard band (LHB) at 1.1 eV below the Fermi level, whereas a Mott-Hubbard band gap of ~1.5 eV is determined from photoluminescence (PL) measurements. These findings provide critical insight into the electronic band structure of YTO and related materials., Comment: 15 pages, 3 figures

One of the challenges of oxide molecular beam epitaxy (MBE) is the synthesis of oxides containing metals with high electronegativity (metals that are hard to oxidize). The use of reactive organometallic precursors can potentially address this issue. To investigate the formation of radicals in MBE, we explored three carefully chosen metal-organic precursors of tin for SnO2 and BaSnO3 growth: tetramethyltin (TMT), tetraethyltin (TET), and hexamethylditin (HMDT). All three precursors produced single-crystalline, atomically smooth, and epitaxial SnO2 (101) films on r-Al2O3 in the presence of an oxygen plasma. The study of growth kinetics revealed reaction-limited and flux-limited regimes except for TET, which also exhibited a decrease in deposition rate with increasing temperature above 800 C. Contrary to these similarities, the performance of these precursors was dramatically different for BaSnO3 growth. TMT and TET were ineffective in supplying adequate tin whereas HMDT yielded phase-pure, stoichiometric BaSnO3 films. Significantly, HMDT resulted in phase-pure and stoichiometric BaSnO3 films even without the use of an oxygen plasma (i.e., with molecular oxygen alone). These results are discussed using the ability of HMDT to form tin radicals and therefore, assisting with Sn to Sn4+ oxidation reaction. Structural and electronic transport properties of films grown using HMDT with and without oxygen plasma are compared. This study provides guideline for the choice of precursors that will enable synthesis of metal oxides containing hard-to-oxidize metals using reactive radicals in MBE., Comment: 18 pages, 6 figures

Quantum corrections to electrical resistance can serve as sensitive probes of the magnetic landscape of a material. For example, interference between time-reversed electron paths gives rise to weak localization effects, which can provide information about the coupling between spins and orbital motion, while the Kondo effect is sensitive to the presence of spin impurities. Here we use low-temperature magnetotransport measurements to reveal a transition from weak antilocalization (WAL) to Kondo scattering in the quasi-two-dimensional electron gas formed at the interface between SrTiO$_3$ and the Mott insulator NdTiO$_3$. This transition occurs as the thickness of the NdTiO$_3$ layer is increased. Analysis of the Kondo scattering and WAL points to the presence of atomic-scale magnetic impurities coexisting with extended magnetic regions that affect transport via a strong magnetic exchange interaction. This leads to distinct magnetoresistance behaviors that can serve as a sensitive probe of magnetic properties in two dimensions., Comment: 5 pages, 3 figures

Reflection high-energy electron diffraction (RHEED) is a ubiquitous in situ molecular beam epitaxial (MBE) characterization tool. Although RHEED can be a powerful means for crystal surface structure determination, it is often used as a static qualitative surface characterization method at discrete intervals during a growth. A full analysis of RHEED data collected during the entirety of MBE growths is made possible using principle component analysis (PCA) and k-means clustering to examine significant boundaries that occur in the temporal clusters grouped from RHEED data and identify statistically significant patterns. This process is applied to data from homoepitaxial SrTiO$_{3}$ growths, heteroepitaxial SrTiO$_{3}$ grown on scandate substrates, BaSnO$_{3}$ films grown on SrTiO$_{3}$ substrates, and LaNiO$_{3}$ films grown on LaAlO$_{3}$ substrates. This analysis may provide additional insights into the surface evolution and transitions in growth modes at precise times and depths during growth, and that video archival of an entire RHEED image sequence may be able to provide more insight and control over growth processes and film quality., Comment: 12 pages, 12 figures

We investigate lanthanum (La) as an n-type dopant in the strain-stabilized tetragonal phase of SrSnO3 grown on GdScO3 (110) using a radical-based hybrid molecular beam epitaxy approach. Fully coherent, epitaxial films with atomically smooth film surface were obtained irrespective of doping density. By combining secondary ion mass spectroscopy and Hall measurements, we demonstrate that each La atom contributes to one electron to the film confirming it occupies Sr-site in SrSnO3 and that it is completely activated. Carrier density exceeding 1 x 10^20 cm-3 was achieved in LSSO films, which is in excellent agreement with the dopant-solubility limit predicted by the density functional theory calculations. A record-high room-temperature mobility of 70 cm2V-1s-1 at 1 x 10^20 cm-3 was obtained in 12 nm La-doped SrSnO3 film making this the thinnest perovskite oxide semiconductor with a reasonably high electron mobility at room temperature. We discuss the structure-dopant-transport property relationships providing essential knowledge for the design of electronic devices using these materials., Comment: 3 figures

A study of the STEM probe channeling in a heterostructures crystalline specimen is presented here with a goal to guide appropriate STEM-based characterization for complex structures. STEM analysis of perovskite BaSnO3/LaAlO3 bilayers is performed and the dominating effects of beam channeling on HAADF- and LAADF-STEM are illustrated. To study the electron beam propagating through BaSnO3/LaAlO3 bilayers, probe intensity depth profiles are calculated, and the effects of probe defocus and atomic column alignment are discussed. Characteristics of the beam channeling are correlated to resulting ADF-STEM images, which is then tested by comparing focal series of plan-view HAADF-STEM images to those recorded experimentally. Additionally, discussions on how to visualize the misfit dislocation network at the BaSnO3/LaAlO3 interface using HAADF- and LAADF-STEM images are provided., Comment: 23 pages, 8 figures

Contrary to the common belief that electron-electron interaction (EEI) should be negligible in s-orbital-based conductors, we demonstrated that the EEI effect could play a significant role on electronic transport leading to the misinterpretation of the Hall data. We show that the EEI effect is primarily responsible for an increase in the Hall coefficient in the La-doped SrSnO3 films below 50 K accompanied by an increase in the sheet resistance. The quantitative analysis of the magnetoresistance (MR) data yielded a large phase coherence length of electrons exceeding 450 nm at 1.8 K and revealed the electron-electron interaction being accountable for breaking of electron phase coherency in La-doped SrSnO3 films. These results while providing critical insights into the fundamental transport behavior in doped stannates also indicate the potential applications of stannates in quantum coherent electronic devices owing to their large phase coherence length., Comment: 3 figures

Through a combination of thin film growth, hard X-ray photoelectron spectroscopy (HAXPES), scanning transmission electron microscopy/electron energy loss spectroscopy (STEM/EELS), magneto-transport measurements, and transport modeling, we report on the demonstration of modulation-doping of BaSnO3 (BSO) using a wider bandgap La-doped SrSnO3 (LSSO) layer. Hard X-ray photoelectron spectroscopy (HAXPES) revealed a valence band offset of 0.71 +/- 0.02 eV between LSSO and BSO resulting in a favorable conduction band offset for remote doping of BSO using LSSO. Nonlinear Hall effect of LSSO/BSO heterostructure confirmed two-channel conduction owing to electron transfer from LSSO to BSO and remained in good agreement with the results of self-consistent solution to one-dimensional Poisson and Schr\"odinger equations. Angle-dependent HAXPES measurements revealed a spatial distribution of electrons over 2-3 unit cells in BSO. These results bring perovskite oxides a step closer to room-temperature oxide electronics by establishing modulation-doping approaches in non-SrTiO3-based oxide heterostructure.

Quantum interference between time-reversed electron paths in two dimensions leads to the well-known weak localization correction to resistance. If spin-orbit coupling is present, the resistance correction is negative, termed weak anti-localization (WAL). Here we report the observation of WAL coexisting with exchange coupling between itinerant electrons and localized magnetic moments. We use low-temperature magneto-transport measurements to investigate the quasi-two-dimensional, high-electron-density interface formed between SrTiO$_3$ (STO) and the anti-ferromagnetic Mott insulator NdTiO$_3$ (NTO). As the magnetic field angle is gradually tilted away from the sample normal, the data reveals the interplay between strong $k$-cubic Rashba-type spin-orbit coupling and a substantial magnetic exchange interaction from local magnetic regions. The resulting quantum corrections to the conduction are in excellent agreement with existing models and allow sensitive determination of the small magnetic moments (22 $\mu_B$ on average), their magnetic anisotropy and mutual coupling strength. This effect is expected to arise in other 2D magnetic materials systems., Comment: 6 pages, 4 figures

The BCS picture of superconductivity describes pairing between electrons originating from a single band. A generalization of this picture occurs in multi-band superconductors, where electrons from two or more bands contribute to superconductivity. The contributions of the different bands can result in an overall enhancement of the critical field and can lead to qualitative changes in the temperature dependence of the upper critical field when compared to the single-band case. While the role of orbital pair-breaking on the critical field of multi-band superconductors has been explored extensively, paramagnetic and spin-orbital scattering effects have received comparatively little attention. Here we investigate this problem using thin films of Nd-doped SrTiO$_3$. We furthermore propose a model for analyzing the temperature-dependence of the critical field in the presence of orbital, paramagnetic and spin-orbital effects, and find a very good agreement with our data. Interestingly, we also observe a dramatic enhancement in the out-of-plane critical field to values well in excess of the Chandrasekhar-Clogston (Pauli) paramagnetic limit, which can be understood as a consequence of multi-band effects in the presence of spin-orbital scattering., Comment: 32 pages

Electronic transport near the insulator-metal transition is investigated in the molecular beam epitaxy-grown SrTiO3/Nd1-xTiO3/SrTiO3 heterostructures using temperature dependent magnetotransport measurements. It was found that Nd-vacancies introduce localized electronic states resulting in the variable range hopping transport at low temperatures. At a fixed Nd-vacancies concentration, a crossover from Mott to Efros-Shklovskii (ES) variable range hopping transport was observed with decreasing temperature. With increasing disorder, a sign reversal of magnetoresistance from positive to negative was observed revealing interplay between intra-state interaction and the energy dependence of the localization length as a function of disorder. These findings highlight the important role of stoichiometry when exploring intrinsic effect using heterostructure and interfaces in addition to offering broad opportunity to tailor low temperature transport using non-stoichiometry defects.

Complex oxide interfaces are a promising platform for studying a wide array of correlated electron phenomena in low-dimensions, including magnetism and superconductivity. The microscopic origin of these phenomena in complex oxide interfaces remains an open question. Here we investigate for the first time the magnetic properties of semi-insulating NdTiO$_3$/SrTiO$_3$ (NTO/STO) interfaces and present the first milli-Kelvin study of NTO/STO. The magnetoresistance (MR) reveals signatures of local ferromagnetic order and of spin-dependent thermally-activated transport, which are described quantitatively by a simple phenomenological model. We discuss possible origins of the interfacial ferromagnetism. In addition, the MR also shows transient hysteretic features on a timescale of ~10-100 seconds. We demonstrate that these are consistent with an extrinsic magneto-thermal origin, which may have been misinterpreted in previous reports of magnetism in STO-based oxide interfaces. The existence of these two MR regimes (steady-state and transient) highlights the importance of time-dependent measurements for distinguishing signatures of ferromagnetism from other effects that can produce hysteresis at low temperatures.

There has been growing interest in perovskite BaSnO3 due to its desirable properties for oxide electronic devices including high electron mobility at room temperature and optical transparency. As these electronic and optical properties originate largely from the electronic structure of the material, here the basic electronic structure of epitaxially-grown BaSnO3 films is studied using high-energy-resolution electron energy-loss spectroscopy in a transmission electron microscope and ab initio calculations. This study provides a detailed description of the dielectric function of BaSnO3, including the energies of bulk plasmon excitations and critical interband electronic transitions, the band structure and partial densities of states, the measured band gap, and more. To make the study representative of a variety of deposition methods, results from BaSnO3 films grown by both hybrid molecular beam epitaxy and high pressure oxygen sputter deposition are reported., Comment: 23 pages, 7 figures, 3 tables

Perovskite oxides form an eclectic class of materials owing to their structural flexibility in accommodating cations of different sizes and valences. They host well known point and planar defects, but so far no line defect has been identified other than dislocations. Using analytical scanning transmission electron microscopy (STEM) and ab initio calculations we have detected and characterized the atomic and electronic structures of a novel line defect in NdTiO3 perovskite. It appears in STEM images as a perovskite cell rotated by 45 degrees. It consists of self-organized Ti-O vacancy lines replaced by Nd columns surrounding a central Ti-O octahedral chain containing Ti4+ ions, as opposed to Ti3+ in the host. The distinct Ti valence in this line defect introduces the possibility of engineering exotic conducting properties in a single preferred direction and tailoring novel desirable functionalities in this Mott insulator., Comment: 24 pages, 5 figures

We have spectroscopically determined the band offsets at epitaxial interfaces of BaSnO3 with SrTiO3(001) and LaAlO3(001). The conduction band minimum is lower in electron energy in the BaSnO3 than in the SrTiO3 and LaAlO3 by 0.6 +/- 0.1 eV and 3.7 +/- 0.1 eV, respectively. Thus, electrons generated in the SrTiO3 and LaAlO3 and transferred to the BaSnO3 by modulation and polarization doping, respectively, are expected to drift under the influence of an electric field without undergoing impurity scattering and the associated loss of mobility. This result bodes well for the realization of oxide-based, high-mobility, two-dimensional electron systems that can operate at ambient temperature.

SrTiO$_{3}$ (STO) epitaxial thin films and heterostructures are of considerable interest due to the wide range of functionalities they exhibit. The alloy perovskite (LaAlO$_{3}$)$_{0.3}$-(Sr$_{2}$AlTaO$_{6}$)$_{0.7}$ (LSAT) is commonly used as a substrate for these material structures due to its structural compatibility with STO and the strain-induced ferroelectric response in STO films grown on LSAT. However, surprisingly little is known about the electronic properties of the STO/LSAT interface despite its potentially important role in affecting the overall electronic structure of system. We examine the band alignment of STO/LSAT heterostructures using x-ray photoelectron spectroscopy for epitaxial STO films deposited using two different molecular beam epitaxy approaches. We find that the valence band offset ranges from +0.2(1) eV to -0.2(1) eV depending on the film surface termination. From these results we extract a conduction band offset from -2.4(1) eV to -2.8(1) eV, indicating that the conduction band edge is more deeply bound in STO and that LSAT will not act as a sink or trap for electrons in the supported film or multilayer., Comment: 14 pages, 3 figures; Accepted in Applied Physics Letters