Search

Recent progress on the signatures of pressure-induced high temperature superconductivity in Ruddlesden Popper (RP) nickelates (Lan+1NinO3n+1) has attracted growing interest in both theoretical calculations and experimental efforts. The fabrication of high-quality single crystalline RP nickelate thin films is critical for possible reducing the superconducting transition pressure and advancing applications in microelectronics in the future. In this study, we report the observations of an active phase transition in RP nickelate films induced by misfit strain. We found that RP nickelate films favor the perovskite structure (n = infinite) under tensile strains, while compressive strains stabilize the La3Ni2O7 (n = 2) phase. The selection of distinct phases is governed by the strain dependent formation energy and electronic configuration. In compressively strained La3Ni2O7, we experimentally determined splitting energy is ~0.2 eV and electrons prefer to occupy in-plane orbitals. First principles calculations unveil a robust coupling between strain effects and the valence state of Ni ions in RP nickelates, suggesting a dual driving force for the inevitable phase co-existence transition in RP nickelates. Our work underscores the sensitivity of RP nickelate formation to epitaxial strain, presenting a significant challenge in fabricating pure-phase RP nickelate films. Therefore, special attention to stacking defects and grain boundaries between different RP phases is essential when discussing the pressure-induced superconductivity in RP nickelates., Comment: 29 pages, 5 figures, one supplementary materials

Releasing the epitaxial oxide heterostructures from substrate constraints leads to the emergence of various correlated electronic phases and paves the way for integrations with advanced semiconductor technologies. Identifying a suitable water-soluble sacrificial layer, compatible with the high-quality epitaxial growth of oxide heterostructures, is currently the key to the development of large-scale freestanding oxide membranes. In this study, we unveil the super-tetragonal Sr4Al2O7 (SAOT) as a promising water-soluble sacrificial layer. The distinct low-symmetric crystal structure of SAOT enables a superior capability to sustain epitaxial strain, thus allowing for broad tunability in lattice constants. The resultant structural coherency and defect-free interface in perovskite ABO3/SAOT heterostructures effectively restrain crack formations during the water-assisted release of freestanding oxide membranes. For a variety of non-ferroelectric oxide membranes, the crack-free areas can span up to a few millimeters in length scale. These compelling features, combined with the inherent high-water solubility, make SAOT a versatile and feasible sacrificial layer for producing high-quality freestanding oxide membranes, thereby boosting their potential for innovative oxide electronics and flexible device designs., Comment: 5 figures and SI, it is the second version of this manuscript

The magnetic correlations at the superconductor/ferromagnet (S/F) interfaces play a crucial role in realizing dissipation-less spin-based logic and memory technologies, such as triplet-supercurrent spin-valves and "{\pi}" Josephson junctions. Here we report the coexistence of an induced large magnetic moment and a crypto ferromagnetic state at high-quality nitride S/F interfaces. Using polarized neutron reflectometry and d. c. SQUID measurements, we quantitatively determined the magnetization profile of S/F bilayer and confirmed the induced magnetic moment in the adjacent superconductor only exists below TC. Interestingly, the direction of the induced moment in the superconductors was unexpectedly parallel to that in the ferromagnet, which contrasts with earlier findings in S/F heterostructures based on metals or oxides. The first-principles calculations verify the observed unusual interfacial spin texture is caused by the Heisenberg direct exchange coupling through d orbital overlapping and severe charge transfer across the interfaces. Our work establishes an incisive experimental probe for understanding the magnetic proximity behavior at S/F interfaces and provides a prototype epitaxial building block for superconducting spintronics., Comment: 21 pages, 5 figures, supplementary file with 14 figures

High-density magnetic memories are key components in spintronics, quantum computing, and energy-efficient electronics. Reduced dimensionality and magnetic domain stability at the nanoscale are essential for the miniaturization of magnetic storage units. Yet, inducing magnetic order, and selectively tuning spin-orbital coupling at specific locations have remained challenging. Here we demonstrate the construction of switchable magnetic nano-islands in a nonmagnetic matrix based on cobaltite homo-structures. The magnetic and electronic states are laterally modified by epitaxial strain, which is regionally controlled by freestanding membranes. Atomically sharp grain boundaries isolate the crosstalk between magnetically distinct regions. The minimal size of magnetic nano-islands reaches 35 nm in diameter, enabling an areal density of 400 Gbit per inch square. Besides providing an ideal platform for precisely controlled read and write schemes, this methodology can enable scalable and patterned memories on silicon and flexible substrates for various applications., Comment: 20 pages,4 figures

Interfaces between transition-metal oxides are able to host two-dimensional electron gases (2DEGs) and exhibit exotic quantum phenomena. Here we report the observation of superconductivity below 230 mK for the heterostructure composed of SrNbO3 (SNO) and SrTiO3 (STO). Different from some other counterparts with two insulators, the metallic SNO provides a novel mechanism to form a quasi 2DEG by charge transfer from bulk towards interface under strain. The superconductivity, residing within the strained SNO layer near the interface, is contributed by an electron system with record-low carrier density. Notably, although embedded in a normal metallic layer with a carrier density 4 to 5 orders higher, the electron system is still uniquely well-protected to retain high mobility and lies deep in extreme quantum regime.

Transition metal nitrides (TMNs) exhibit fascinating physical properties that hold great potential in future device applications. To stack two-dimensional TMNs with other functional materials that have dissimilar orientations and symmetries requires to separate epitaxial TMNs from the growth substrates. However, the lattice constants of TMNs are not compatible with those of most sacrificial layers, leading to a great challenge to fabricate high-quality single crystalline TMN membranes. In this letter, we report the application of a water-soluble BaO sacrificial layer as a general approach to create freestanding TMN membranes. Taken CrN as an example, the relatively small lattice mismatch and identical cubic structure between BaO and CrN ensure the growth of heterostructures. Millimeter-size CrN membrane allows us to directly observe the planar-view of atomic structure and to correlate its electronic state with intrinsic transport properties. Our work provides the opportunity to fabricate freestanding TMN membranes and the ability to transfer them to arbitrary substrates. The integration of TMN membranes with other materials will stimulate further studies in the emergent phenomena at heterointerfaces., Comment: 16 pages; 3 figures

Interfacial magnetism stimulates the discovery of giant magnetoresistance and spin-orbital coupling across the heterointerfaces, facilitating the intimate correlation between spin transport and complex magnetic structures. Over decades, functional heterointerfaces composed of nitrides are seldomly explored due to the difficulty in synthesizing high-quality and correct composition nitride films. Here we report the fabrication of single-crystalline ferromagnetic Fe3N thin films with precisely controlled thickness. As film thickness decreasing, the magnetization deteriorates dramatically, and electronic state transits from metallic to insulating. Strikingly, the high-temperature ferromagnetism maintains in a Fe3N layer with a thickness down to 2 u. c. (~ 8 {\AA}). The magnetoresistance exhibits a strong in-plane anisotropy and meanwhile the anomalous Hall resistance reserves its sign when Fe3N layer thickness exceeds 5 u. c. Furthermore, we observe a sizable exchange bias at the interfaces between a ferromagnetic Fe3N and an antiferromagnetic CrN. The exchange bias field and saturation moment strongly depend on the controllable bending curvature using cylinder diameter engineering (CDE) technique, implying the tunable magnetic states under lattice deformation. This work provides a guideline for exploring functional nitride films and applying their interfacial phenomena for innovative perspectives towards the practical applications.

Interfaces formed by correlated oxides offer a critical avenue for discovering emergent phenomena and quantum states. However, the fabrication of oxide interfaces with variable crystallographic orientations and strain states integrated along a film plane is extremely challenge by conventional layer-by-layer stacking or self-assembling. Here, we report the creation of morphotropic grain boundaries (GBs) in laterally interconnected cobaltite homostructures. Single-crystalline substrates and suspended ultrathin freestanding membranes provide independent templates for coherent epitaxy and constraint on the growth orientation, resulting in seamless and atomically sharp GBs. Electronic states and magnetic behavior in hybrid structures are laterally modulated and isolated by GBs, enabling artificially engineered functionalities in the planar matrix. Our work offers a simple and scalable method for fabricating unprecedented innovative interfaces through controlled synthesis routes as well as provides a platform for exploring potential applications in neuromorphics, solid state batteries, and catalysis., Comment: 38 pages, 4 main figures

Emergent phenomena at heterointerfaces are directly associated with the bonding geometry of adjacent layers. Effective control of accessible parameters, such as the bond length and bonding angles, offers an elegant method to tailor competing energies of the electronic and magnetic ground states. In this study, we construct unit thick syntactic layers of cobaltites within a strongly tilted octahedral matrix via atomically precise synthesis. The octahedral tilt patterns of adjacent layers propagate into cobaltites, leading to a continuation of octahedral tilting while maintaining significant misfit tensile strain. These effects induce severe rumpling within an atomic plane of neighboring layers triggers the electronic reconstruction between the splitting orbitals. First-principles calculations reveal that the cobalt ions transits to a higher spin state level upon octahedral tilting, resulting in robust ferromagnetism in ultrathin cobaltites. This work demonstrates a design methodology for fine-tuning the lattice and spin degrees of freedom in correlated quantum heterostructures by exploiting epitaxial geometric engineering., Comment: 18 pages, 5 figures

Misfit strain delivered from single-crystal substrates typically modifies the ground states of transition metal oxides, generating increasing interests in designing modern transducers and sensors. Here, we demonstrate that magnetotransport properties of La$_{0.67}$Sr$_{0.33}$MnO$_3$ (LSMO) films were continuously tuned by uniaxial strain produced by a home-designed bending jig. The electrical conductivity and Curie temperature of LSMO films are enhanced by bending stresses. The resistivity of a u-shape bended LSMO decays three times faster than that of a n-shape bended LSMO as a response to the same magnitude of strain. The asymmetric magnetic states in uniaxially strained LSMO are attributed to the dual actions of Jahn-Teller distortion and strain gradient mediated flexoelectric fields in an adjacent ferroelectric layer. These findings of multi-field regulation in a single material provide a feasible means for developing flexible electronic and spintronic devices., Comment: 17 pages, 4 figures

Two-dimensional electron gas (2DEG) formed at the interface between two insulating oxides offers an opportunity for fundamental research and device applications. Binary alkaline earth metal oxides possess compatible lattice constants with both silicon and perovskite oxides, exhibiting an enormous potential to bridging those two materials classes for multifunctionalities. Here we report the formation of 2DEG at the interface between the rock-salt BaO and SrTiO3. The highest electron mobility reaches 69000 cm^2 V.S^-1 at 2 K, leading to the typical Shubniko de Haas (SdH) oscillations under the high magnetic fields. The presence of SdH oscillations at different field-angles reveals a quasi-two-dimensional character of the Fermi surface. The first-principles calculations suggest that the effective charge transfer from the BaO to Ti 3dxy orbital at the interfaces is responsible to the observed high carrier mobility. Our results demonstrate that the BaO/STO heterointerface is a platform for exploring the correlated quantum phases, opening a door to the low-power and mesoscopic electronic devices., Comment: 18 pages; 5 figures

Heterointerfaces have led to the discovery of novel electronic and magnetic states because of their strongly entangled electronic degrees of freedom. Single-phase chromium compounds always exhibit antiferromagnetism following the prediction of Goodenough-Kanamori rules. So far, exchange coupling between chromium ions via hetero-anions has not been explored and the associated quantum states is unknown. Here we report the successful epitaxial synthesis and characterizations of chromium oxide (Cr2O3)-chromium nitride (CrN) superlattices. Room-temperature ferromagnetic spin ordering is achieved at the interfaces between these two antiferromagnets, and the magnitude of the effect decays with increasing layer thickness. First-principles calculations indicate that robust ferromagnetic spin interaction between Cr3+ ions via anion-hybridizations across the interface yields the lowest total energy. This work opens the door to fundamental understanding of the unexpected and exceptional properties of oxide-nitride interfaces and provides access to hidden phases at low-dimensional quantum heterostructures., Comment: 21 pages, 4 figures

Electronic phase transition in strongly correlated materials is extremely sensitive to the dimensionality and crystallographic orientations. Transition metal nitrides (TMNs) are seldom investigated due to the difficulty in fabricating the high-quality and stoichiometric single crystals. In this letter, we report the epitaxial growth and electronic properties of CrN films on different-oriented NdGaO3 (NGO) substrates. Astonishingly, the CrN films grown on (110)-oriented NGO substrates maintain a metallic phase, whereas the CrN films grown on (010)-oriented NGO substrates are semiconducting. We attribute the unconventional electronic transition in the CrN films to the strongly correlation with epitaxial strain. The effective modulation of bandgap by the anisotropic strain triggers the metal-to-insulator transition consequently. This work provides a convenient approach to modify the electronic ground states of functional materials using anisotropic strain and further stimulates the investigations of TMNs.

Orientation control of oxygen vacancy channel (OVC) is a highly desirable for tailoring oxygen diffusion as it serves fast transport channel in ion conductors, which is widespread exploited in solid-state fuel cells, catalysts, and ion-batteries. Direct observation of oxygen-ions hopping towards preferential vacant sites is a key to clarifying migration pathways. Here we report the anisotropic oxygen-ion migration mediated by strain in ultrathin cobaltites via in-situ thermal activation in an atomic-resolved transmission electron microscopy. Oxygen migration pathways are constructed on the basis of the atomic structure during the OVC switching, which is manifested as the vertical-to-horizontal OVC switching under tensile strain, but the horizontal-to-diagonal switching under compression. We evaluate the topotactic structural changes to OVC, determine the crucial role of tolerance factor for OVC stability and establish the strain-dependent phase diagram. Our work provides a practical guide for engineering OVC orientation that is applicable ionic-oxide electronics.

Control of magnetic states by external factors has garnered a mainstream status in spintronic research for designing low power consumption and fast-response information storage and processing devices. Previously, magnetic-cation substitution is the conventional means to induce ferromagnetism in an intrinsic antiferromagnet. Theoretically, the anion-doping is proposed to be another effect means to change magnetic ground states. Here we demonstrate the synthesis of high-quality single-phase chromium oxynitride thin films using in-situ nitrogen doping. Unlike antiferromagnetic monoanionic chromium oxide and nitride phases, chromium oxynitride exhibits a robust ferromagnetic and insulating state, as demonstrated by the combination of multiple magnetization probes and theoretical calculations. With increasing the nitrogen content, the crystal structure of chromium oxynitride transits from trigonal (R3c) to tetragonal (4mm) phase and its saturation magnetization reduces significantly. Furthermore, we achieve a large and controllable exchange bias field in the chromia heterostructures by synthetic anion engineering. This work reflects the anion engineering in functional oxides towards the potential applications in giant magnetoresistance and tunnelling junctions of modern magnetic sensors and read heads.

Electronic states of a correlated material can be effectively modified by structural variations delivered from a single-crystal substrate. In this letter, we show that the CrN films grown on MgO (001) substrates have a (001) orientation, whereas the CrN films on {\alpha}-Al2O3 (0001) substrates are oriented along (111) direction parallel to the surface normal. Transport properties of CrN films are remarkably different depending on crystallographic orientations. The critical thickness for the metal-insulator transition (MIT) in CrN 111 films is significantly larger than that of CrN 001 films. In contrast to CrN 001 films without apparent defects, scanning transmission electron microscopy results reveal that CrN 111 films exhibit strain-induced structural defects, e. g. the periodic horizontal twinning domains, resulting in an increased electron scattering facilitating an insulating state. Understanding the key parameters that determine the electronic properties of ultrathin conductive layers is highly desirable for future technological applications., Comment: 19 pages, 4 figures

Manipulation of octahedral distortion at atomic length scale is an effective means to tune the physical ground states of functional oxides. Previous work demonstrates that epitaxial strain and film thickness are variable parameters to modify the octahedral rotation and tilt. However, selective control of bonding geometry by structural propagation from adjacent layers is rarely studied. Here we propose a new route to tune the ferromagnetic response in SrRuO3 (SRO) ultrathin layers by oxygen coordination of adjacent SrCuO2 (SCO) layers. The infinite-layered CuO2 in SCO exhibits a structural transformation from "planar-type" to "chain-type" as reducing film thickness. These two orientations dramatically modify the polyhedral connectivity at the interface, thus altering the octahedral distortion of SRO. The local structural variation changes the spin state of Ru and hybridization strength between Ru 4d and O 2p orbitals, leading to a significant change in the magnetoresistance and anomalous Hall resistivity of SRO layers. These findings could launch further investigations into adaptive control of magnetoelectric properties in quantum oxide heterostructures using oxygen coordination.