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We investigate the effect of strain and film thickness on the orbital and magnetic properties of ${\mathrm{LaSrCrO}}_{3}\phantom{\rule{0.16em}{0ex}}(\mathrm{LSCO})/{\mathrm{LaSrMnO}}_{3}$ (LSMO) heterostructures using bulk magnetometry, soft x-ray magnetic spectroscopy, first-principles density-functional theory, high-resolution electron microscopy, and x-ray diffraction. We observe an antiparallel ordering of the magnetic moments between the ferromagnetic LSMO layers and the LSCO spacers, leading to a strain-independent ferromagnetic ground state of the LSCO/LSMO heterostructures for LSMO layers as thin as two unit cells. As the LSMO thickness is increased, a net ferromagnetic state is maintained, however, the average magnetic moment per Mn is found to be dependent on the magnitude of the substrate-induced strain. The differences in the magnetic responses are related to preferential occupation of the Mn ${x}^{2}\ensuremath{-}{y}^{2}$ (in-plane) $d$ orbitals for tensile strain and $3{z}^{2}\ensuremath{-}{r}^{2}$ (out-of-plane) orbitals under compressive strain, leading to competing ferromagnetic and antiferromagnetic exchange interactions within the LSMO layers. These results underscore the relative contributions of orbital, structural, and spin degrees of freedom and their tunability in atomically thin crystalline complex oxide layers.

The control of chemical exchange across heterointerfaces formed between ultrathin functional transition-metal oxide layers provides an effective route to manipulate the electronic properties of these systems. By determining the layer-resolved structural profile across the interface between the Mott insulator, LaTiO3 (LTO) grown epitaxially on SrTiO3 (STO)-buffered silicon by molecular beam epitaxy, we find that interfacial cationic exchange depends on the surface termination of the strained STO buffer. Using a combination of temperature-dependent transport and synchrotron x-ray crystal truncation rods and reciprocal space mapping, an enhanced conductivity in STO/LTO/SrO-terminated STO buffers compared to heterostructures with TiO 2-terminated STO buffers is correlated with La/Sr exchange and the formation of metallic La 1−xSr xTiO 3. La/Sr exchange effectively reduces the strain energy of the system due to the large lattice mismatch between the nominal oxide layers and the Si substrate.

A single atomic layer of ZrO2 exhibits ferroelectric switching behavior when grown with an atomically abrupt interface on silicon. Hysteresis in capacitance–voltage measurements of a ZrO2 gate stack demonstrate that a reversible polarization of the ZrO2 interface structure couples to the carriers in the silicon. First-principles computations confirm the existence of multiple stable polarization states and the energy shift in the semiconductor electron states that result from switching between these states. This monolayer ferroelectric represents a new class of materials for achieving devices that transcend conventional complementary metal oxide semiconductor (CMOS) technology. Significantly, a single atomic layer ferroelectric allows for more aggressively scaled devices than bulk ferroelectrics, which currently need to be thicker than 5–10 nm to exhibit significant hysteretic behavior (Park, et al. Adv. Mater. 2015, 27, 1811).

Complex oxides and semiconductors exhibit distinct yet complementary properties owing to their respective ionic and covalent natures. By electrically coupling complex oxides to traditional semiconductors within epitaxial heterostructures, enhanced or novel functionalities beyond those of the constituent materials can potentially be realized. Essential to electrically coupling complex oxides to semiconductors is control of the physical structure of the epitaxially grown oxide, as well as the electronic structure of the interface. Here we discuss how composition of the perovskite A- and B-site cations can be manipulated to control the physical and electronic structure of semiconductor—complex oxide heterostructures. Two prototypical heterostructures, Ba1−xSrxTiO3/Ge and SrZrxTi1−xO3/Ge, will be discussed. In the case of Ba1−xSrxTiO3/Ge, we discuss how strain can be engineered through A-site composition to enable the re-orientable ferroelectric polarization of the former to be coupled to carriers in the semiconductor. In the case of SrZrxTi1−xO3/Ge we discuss how B-site composition can be exploited to control the band offset at the interface. Analogous to heterojunctions between compound semiconducting materials, control of band offsets, i.e., band-gap engineering, provides a pathway to electrically couple complex oxides to semiconductors to realize a host of functionalities.

The strong interfacial coupling at the 3d-5d transition metal-oxide interfaces has generated excitement due to the possibility of engineering a wide range of quantum phenomena and functionalities. Here, we investigate the electronic interfacial coupling and structural properties of LaCrO3/KTaO3 heterostructures. High-quality LaCrO3 films were grown on KTaO3 substrates using molecular beam epitaxy. These heterostructures show a robust two-dimensional electron gas and a metallic behavior down to liquid helium temperature. Using magnetoresistance measurements, we analyze the coupling of electronic orders between Cr 3d and Ta 5d states and observe signatures of weak anti-localization and Kondo scattering at low-temperature transport. The results provide direct evidence that a crossover (weak anti-localization to Kondo) occurs with increasing temperature as the dephasing scattering events reduce the coherence length. Our observations allow for a clear and detailed picture of two distinct quantum corrections to conductivity at low temperature.

We investigate the structural and magnetic properties of La 0.7 Sr 0.3 CrO 3 ( LSCO ) / La 0.7 Sr 0.3 MnO 3 (LSMO) heterostructures grown on (001)-oriented MgO by molecular beam epitaxy. Due to the large film-substrate lattice mismatch, strain relaxation is found to occur within the first 2–3 unit cells (uc) of the film as evidenced by reflection high energy electron diffraction and high-resolution synchrotron x-ray reciprocal space mapping. We find that the presence of the LSCO spacer and capping layers leads to ferromagnetism in ultra-thin LSMO layers with thicknesses of the order of 2 uc with the magnetic easy axis oriented in the film plane. Net magnetic moments of 1.4 and 2.4 μ B / Mn are measured for (2 uc LSCO/2 uc LSMO) and (2 uc LSCO/4 uc LSMO) superlattices, respectively, by superconducting quantum interference device magnetometry. The effective magnetic anisotropy of the relaxed (2 uc LSCO/4 uc LSMO) heterostructure is found to be an order of magnitude higher than bulk LSMO highlighting the critical role of interfacial interactions in tuning magnetic anisotropy at complex oxide interfaces.

Complex oxides and semiconductors exhibit distinct yet complementary properties owing to their respective ionic and covalent natures. By electrically coupling oxides to semiconductors within epitaxial heterostructures, enhanced or novel functionalities beyond those of the constituent materials can potentially be realized. Key to electrically coupling oxides to semiconductors is controlling the physical and electronic structure of semiconductor – crystalline oxide heterostructures. Here we discuss how composition of the oxide can be manipulated to control physical and electronic structure in Ba1-xSrxTiO3/ Ge and SrZrxTi1-xO3/Ge heterostructures. In the case of the former we discuss how strain can be engineered through composition to enable the re-orientable ferroelectric polarization to be coupled to carriers in the semiconductor. In the case of the latter we discuss how composition can be exploited to control the band offset at the semiconductor - oxide interface. The ability to control the band offset, i.e. band-gap engineering, provides a pathway to electrically couple crystalline oxides to semiconductors to realize a host of functionalities.

The relationship between the sheet carrier concentration, ns, of LaCrO3(LCO)/SrTiO3(STO) heterostructures and their structural properties has been investigated. Under low oxygen partial pressure, the STO substrate is reduced during growth as evidenced by a high ns of 1016 cm−2. By controlling the post-growth annealing conditions, heterostructures with ns of 1013–1016 cm−2 are achieved. The atomic-scale structure of the samples is obtained using high-resolution synchrotron x-ray diffraction measurements. For heterostructures with ns at or below 3 × 1013 cm−2, polar distortions are present within the LCO layers and increase in magnitude with a decrease in sheet carrier concentration. These distortions are absent for samples with ns on the order of 1015–1016 cm−2 where interfacial carriers play a role in alleviating the polar discontinuity at the LCO/STO interface. These results suggest that interfacial charge carriers and polar distortions can act as complementary mechanisms to alleviate the polar discontinuity at polar/non-polar complex oxide interfaces.

In the recent past, heterostructures of magnetic oxide thin films have attracted a great deal of research excitement due to very interesting physical properties such as antiferromagnetic interlayer coupling, tunable exchange-bias, interfacial driven magnetic properties and high mobility electron gas across the interfaces. In this work, we report on the comprehensive magnetic properties observed from the heterostructures of (2 unit cells) La0.7Sr0.3CrO3/(8 unit cells) La0.7Sr0.3MnO3/(2 unit cells) La0.7Sr0.3CrO3, which are epitaxially deposited on SrTiO3 substrate by plasma-assisted oxide molecular beam epitaxy. Using SQUID magnetometer, the magnetic properties are studied when the magnetic field was applied both in plane and out of plane. The Curie temperature of this structure is found to be at 290 K. Most significantly, at 2 K, we observed a complete up/down shift (along magnetization axis) of hysteresis loop when the sample was cooled under a magnetic field of ± 5000 Oe in the in-plane configuration. We believe that the strong antiferromagnetic (super) exchange coupling of Mn-Cr across the two interfaces is responsible for the observed exchange bias. We will present and discuss our in-detailed experimental findings collected on this heterostructure as a function of temperature and magnetic field.

The interfacial structure of SrZrxTi1−xO3 films grown on semiconducting Ge substrates is investigated by synchrotron X-ray diffraction and first-principles density functional theory. By systematically tuning the Zr content x, the effects of bonding at the interface and epitaxial strain on the physical structure of the film can be distinguished. The interfacial perovskite layers are found to be polarized as a result of cation-anion ionic displacements perpendicular to the perovskite/semiconductor interface. We find a correlation between the observed buckling and valence band offsets at the SrZrxTi1−xO3/Ge interface. The trends in the theoretical valence band offsets as a function of Zr content for the polar structures are in agreement with reported X-ray photoelectron spectroscopy measurements. These results have important implications for the integration of functional oxide materials with established semiconductor based technologies.

Electronic, lattice, and spin interactions at the interfaces between crystalline complex transition metal oxides can give rise to a wide range of functional electronic and magnetic phenomena not found in bulk. At hetero-interfaces, these interactions may be enhanced by combining oxides where the polarity changes at the interface. The physical structure between non-polar SrTiO$_3$ and polar La$_{1-x}$Sr$_x$MnO$_3$(x=0.2) is investigated using high resolution synchrotron x-ray diffraction to directly determine the role of structure in compensating the polar discontinuity. At both the oxide-oxide interface and vacuum-oxide interfaces, the lattice is found to expand and rumple along the growth direction. The SrTiO$_3$/La$_{1-x}$Sr$_x$MnO$_3$ interface also exhibits intermixing of La and Sr over a few unit cells. The results, hence, demonstrate that polar distortions and ionic intermixing coexist and both pathways play a significant role at interfaces with polar discontinuities.

The effect of growth conditions on the structural and electronic properties of the polar/non-polar LaCrO$_3$/SrTiO$_3$ (LCO/STO) interface has been investigated. The interface is either insulating or metallic depending on growth conditions. A high sheet carrier concentration of 2x10$^{16}$ cm$^{-2}$ and mobility of 30,000 cm$^2$/V s is reported for the metallic interfaces, which is similar to the quasi-two dimensional gas at the LaAlO$_{3}$/SrTiO$_{3}$ interface with similar growth conditions. High-resolution synchrotron X-ray-based structural determination of the atomic-scale structures of both metallic and insulating LCO/STO interfaces show chemical intermixing and an interfacial lattice expansion. Angle resolved photoemission spectroscopy of 2 and 4 uc metallic LCO/STO shows no intensity near the Fermi level indicating that the conducting region is occurring deep enough in the substrate to be inaccessible to photoemission spectroscopy. Post-growth annealing in flowing oxygen causes a reduction in the sheet carrier concentration and mobility for the metallic interface while annealing the insulating interface at high temperatures and low oxygen partial pressures results in metallicity. These results highlight the critical role of defects related to oxygen vacancies on the creation of mobile charge carriers at the LCO/STO heterointerface.

We determine the surface reconstruction of $\mathrm{SrTi}{\mathrm{O}}_{3}$ used to achieve superconducting FeSe films in experiments, which is different from the $1\ifmmode\times\else\texttimes\fi{}1\mathrm{Ti}{\mathrm{O}}_{2}$-terminated $\mathrm{SrTi}{\mathrm{O}}_{3}$ assumed by most previous theoretical studies. In particular, we identify the existence of a double $\mathrm{Ti}{\mathrm{O}}_{2}$ layer at the FeSe/$\mathrm{SrTi}{\mathrm{O}}_{3}$ interface that plays two important roles. First, it facilitates the epitaxial growth of FeSe. Second, ab initio calculations reveal a strong tendency for electrons to transfer from an oxygen deficient $\mathrm{SrTi}{\mathrm{O}}_{3}$ surface to FeSe when the double $\mathrm{Ti}{\mathrm{O}}_{2}$ layer is present. The double layer helps to remove the hole pocket in the FeSe at the \ensuremath{\Gamma} point of the Brillouin zone and leads to a band structure characteristic of superconducting samples. The characterization of the interface structure presented here is a key step towards the resolution of many open questions about this superconductor.

The strong interaction at an interface between a substrate and thin film leads to epitaxy and provides a means of inducing structural changes in the epitaxial film. These induced material phases often exhibit technologically relevant electronic, magnetic, and functional properties. The 2×1 surface of a Ge(001) substrate applies a unique type of epitaxial constraint on thin films of the perovskite oxide BaTiO_{3} where a change in bonding and symmetry at the interface leads to a non-bulk-like crystal structure of the BaTiO_{3}. While the complex crystal structure is predicted using first-principles theory, it is further shown that the details of the structure are a consequence of hidden phases found in the bulk elastic response of the BaTiO_{3} induced by the symmetry of forces exerted by the germanium substrate.

We present electrical and structural characterization of epitaxial LaTiO3/SrTiO3 heterostructures integrated directly on Si(100). By reducing the thicknesses of the heterostructures, an enhancement in carrier-carrier scattering is observed in the Fermi liquid behavior, followed by a metal to insulator transition in the electrical transport. The insulating behavior is described by activated transport, and its onset occurs near an occupation of 1 electron per Ti site within the SrTiO3, providing evidence for a Mott driven transition. We also discuss the role that structure and gradients in strain could play in enhancing the carrier density. The manipulation of Mott metal-insulator behavior in oxides grown directly on Si opens the pathway to harnessing strongly correlated phenomena in device technologies.

We describe a general materials design approach that produces large orbital energy splittings (orbital polarization) in nickelate heterostructures, creating a two-dimensional single-band electronic surface at the Fermi energy. The resulting electronic structure mimics that of the high temperature cuprate superconductors. The two key ingredients are: (i) the construction of atomic-scale distortions about the Ni site via charge transfer and internal electric fields, and (ii) the use of three component (tri-component) superlattices to break inversion symmetry. We use {\it ab initio} calculations to implement the approach, with experimental verification of the critical structural motif that enables the design to succeed., Comment: 12 pages, 3 figures and 1 table

In recent years, epitaxial growth of self-assembled quantum dots has offered a way to incorporate new properties into existing solid state devices. Although the droplet heteroepitaxy method is relatively complex, it is quite relaxed with respect to the material combinations that can be used. This offers great flexibility in the systems that can be achieved. In this paper we review the structure and composition of a number of quantum dot systems grown by the droplet heteroepitaxy method, emphasizing the insights that these experiments provide with respect to the growth process. Detailed structural and composition information has been obtained using surface X-ray diffraction analyzed by the COBRA phase retrieval method. A number of interesting phenomena have been observed: penetration of the dots into the substrate (“nano-drilling”) is often encountered; interdiffusion and intermixing already start when the group III droplets are deposited, and structure and composition may be very different from the one initially intended.

International audience; The authors use Fresnel diffraction from knife-edges to demonstrate the spatial coherence of a tabletop ultrafast x-ray source produced by laser-plasma interaction. Spatial coherence is achieved in the far field by producing micrometer-scale x-ray spot dimensions. The results show an x-ray source size of 6 μm that leads to a transversal coherence length of 20 μm at a distance of 60 cm from the source. Moreover, they show that the source size is limited by the spatial spread of the absorbed laser energy.