Strain-Engineered Metal-to-Insulator Transition and Orbital Polarization in Nickelate Superlattices Integrated on Silicon

Epitaxial growth of SrTiO3 (STO) on silicon greatly accelerates the monolithic integration of multifunctional oxides into the mainstream semiconductor electronics. However, oxide superlattices (SLs), the birthplace of many exciting discoveries, remain largely unexplored on silicon. In this work, LaNiO3/LaFeO3 SLs are synthesized on STO-buffered silicon (Si/STO) and STO single-crystal substrates, and their electronic properties are compared using dc transport and X-ray absorption spectroscopy. Both sets of SLs show a similar thickness-driven metal-to-insulator transition, albeit with resistivity and transition temperature modified by the different amounts of strain. In particular, the large tensile strain promotes a pronounced Ni (Formula presented.) orbital polarization for the SL grown on Si/STO, comparable to that reported for LaNiO3 SL epitaxially strained to DyScO3 substrate. Those results illustrate the ability to integrate oxide SLs on silicon with structure and property approaching their counterparts grown on STO single crystal, and also open up new prospects of strain engineering in functional oxides based on the Si platform. © 2020 The Authors. Advanced Materials published by Wiley-VCH Gmb

Integration of Single Oriented Oxide Superlattices on Silicon Using Various Template Techniques

To benefit from the diverse functionalities of perovskite oxides in silicon-based complementary metal oxide semiconductor (CMOS) technology, integrating oxides into a silicon platform has become one of the major tasks for oxide research. Using the deposition of LaMnO3/SrTiO3 (STO) superlattices (SLs) as a case study, we demonstrate that (001) single oriented oxide SLs can be integrated on Si using various template techniques, including a single-layer buffer of STO prepared by molecular beam epitaxy (MBE) and pulsed laser deposition, a multilayer buffer of Y-stabilized zirconia/CeO2/LaNiO3/STO, and STO-coated two-dimensional nanosheets of Ca2Nb3O10 (CNO) and reduced graphene oxide. The textured SL grown on STO-coated CNO nanosheets shows the highest crystallinity, owing to the small lattice mismatch between CNO and STO as well as less clamping from a Si substrate. The epitaxial SL grown on STO buffer prepared by MBE suffers the largest thermal strain, giving rise to a strongly suppressed saturation magnetization but an enhanced coercive field, as compared to the reference SL grown on an STO single crystal. These optional template techniques used for integrating oxides on Si are of significance to fulfill practical applications of oxide films in different fields

Thermal-strain-engineered ferromagnetism of LaMnO3/SrTiO3 heterostructures grown on silicon

The integration of oxides on Si remains challenging, which largely hampers the practical applications of oxide-based electronic devices with superior performance. Recently, LaMnO3/SrTiO3 (LMO/STO) heterostructures have gained renewed interest for the debating origin of the ferromagnetic-insulating ground state as well as for their spin-filter applications. Here we report on the structural and magnetic properties of high-quality LMO/STO heterostructures grown on silicon. The chemical abruptness across the interface was investigated by atomic-resolution scanning transmission electron microscopy. The difference in the thermal expansion coefficients between LMO and Si imposed a large biaxial tensile strain to the LMO film, resulting in a tetragonal structure with c/a∼0.983. Consequently, we observed a significantly suppressed ferromagnetism along with an enhanced coercive field, as compared to the less distorted LMO film (c/a∼1.004) grown on STO single crystal. The results are discussed in terms of tensile-strain enhanced antiferromagnetic instabilities. Moreover, the ferromagnetism of LMO on Si sharply disappeared below a thickness of 5 unit cells, in agreement with the LMO/STO case, pointing to a robust critical behavior irrespective of the strain state. Our results demonstrate that the growth of oxide films on Si can be a promising way to study the tensile-strain effects in correlated oxides, and also pave the way towards the integration of multifunctional oxides on Si with atomic-layer control

Integration of Single Oriented Oxide Superlattices on Silicon Using Various Template Techniques

To benefit from the diverse functionalities of perovskite oxides in silicon-based complementary metal oxide semiconductor (CMOS) technology, integrating oxides into a silicon platform has become one of the major tasks for oxide research. Using the deposition of LaMnO3/SrTiO3 (STO) superlattices (SLs) as a case study, we demonstrate that (001) single oriented oxide SLs can be integrated on Si using various template techniques, including a single-layer buffer of STO prepared by molecular beam epitaxy (MBE) and pulsed laser deposition, a multilayer buffer of Y-stabilized zirconia/CeO2/LaNiO3/STO, and STO-coated two-dimensional nanosheets of Ca2Nb3O10 (CNO) and reduced graphene oxide. The textured SL grown on STO-coated CNO nanosheets shows the highest crystallinity, owing to the small lattice mismatch between CNO and STO as well as less clamping from a Si substrate. The epitaxial SL grown on STO buffer prepared by MBE suffers the largest thermal strain, giving rise to a strongly suppressed saturation magnetization but an enhanced coercive field, as compared to the reference SL grown on an STO single crystal. These optional template techniques used for integrating oxides on Si are of significance to fulfill practical applications of oxide films in different fields

Strain-Engineered Metal-to-Insulator Transition and Orbital Polarization in Nickelate Superlattices Integrated on Silicon

Epitaxial growth of SrTiO3 (STO) on silicon greatly accelerates the monolithic integration of multifunctional oxides into the mainstream semiconductor electronics. However, oxide superlattices (SLs), the birthplace of many exciting discoveries, remain largely unexplored on silicon. In this work, LaNiO3/LaFeO3 SLs are synthesized on STO-buffered silicon (Si/STO) and STO single-crystal substrates, and their electronic properties are compared using dc transport and X-ray absorption spectroscopy. Both sets of SLs show a similar thickness-driven metal-to-insulator transition, albeit with resistivity and transition temperature modified by the different amounts of strain. In particular, the large tensile strain promotes a pronounced Ni (Formula presented.) orbital polarization for the SL grown on Si/STO, comparable to that reported for LaNiO3 SL epitaxially strained to DyScO3 substrate. Those results illustrate the ability to integrate oxide SLs on silicon with structure and property approaching their counterparts grown on STO single crystal, and also open up new prospects of strain engineering in functional oxides based on the Si platform. © 2020 The Authors. Advanced Materials published by Wiley-VCH Gmb

Signatures of enhanced out-of-plane polarization in asymmetric BaTiO3 superlattices integrated on silicon

In order to bring the diverse functionalities of transition metal oxides into modern electronics, it is imperative to integrate oxide films with controllable properties onto the silicon platform. Here, we present asymmetric LaMnO3/BaTiO3/SrTiO3 superlattices fabricated on silicon with layer thickness control at the unit-cell level. By harnessing the coherent strain between the constituent layers, we overcome the biaxial thermal tension from silicon and stabilize c-axis oriented BaTiO3 layers with substantially enhanced tetragonality, as revealed by atomically resolved scanning transmission electron microscopy. Optical second harmonic generation measurements signify a predominant out-of-plane polarized state with strongly enhanced net polarization in the tricolor superlattices, as compared to the BaTiO3 single film and conventional BaTiO3/SrTiO3 superlattice grown on silicon. Meanwhile, this coherent strain in turn suppresses the magnetism of LaMnO3 as the thickness of BaTiO3 increases. Our study raises the prospect of designing artificial oxide superlattices on silicon with tailored functionalities.ISSN:2041-172

Direct observation of the electronic states of photoexcited hematite with ultrafast 2p3d X-ray absorption spectroscopy and resonant inelastic X-ray scattering

Hematite, α-Fe2O3, is an important semiconductor for photoelectrochemical water splitting. Its low charge carrier mobility and the presence of midgap states provide favourable conditions for electron-hole recombination, hence affecting the semiconductor's photoelectrochemical efficiency. The nature of the excited state and charge carrier transport in hematite is strongly debated. In order to further understand the fundamental properties of the hematite photoexcited state, we conducted femtosecond 2p (L3) X-ray absorption (XAS) and 2p3d resonant inelastic scattering (RIXS) measurements on hematite thin-films at the Pohang Accelerator Laboratory X-ray Free Electron Laser (PAL-XFEL). The observed spectral changes and kinetic processes are in agreement with previous 3p XAS reports. The potential additional information that could be acquired from 2p3d RIXS experiments is also discussed