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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

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.

A variety of emergent phenomena has been enabled by interface engineering in the complex oxides heterostructures. While extensive attention has been attracted to LaMnO3 (LMO) thin films for observing the control of functionalities at its interface with substrate, the nature of the magnetic phases in the thin film is, however,controversial. Here, it is reported that the ferromagnetism in 2 and 5 unit cells thick LMO films epitaxially deposited (001)-SrTiO3 substrates ferromagnetic/ferromagnetic coupling in 8 and 10-unit-cell ones, and a striking ferromagnetic/antiferromagnetic pinning effect with apparent positive exchange bias in 15 and 20-unit-cell ones are observed. This novel phenomenon in both 15 and 20-unit-cell films indicates a coexistence of three magnetic orderings in a single LMO film.The high-resolution scanning transmission electron microscopy suggests a P21/n to Pbnm symmetry transition from interface to surface, with the spatial stratification of MnO6 octahedral morphology, corresponding to different magnetic orderings. These results should shed some new lights on manipulating the functionality of oxides by interface engineering., Comment: 15 pages, 4 figures

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.

Low-dimensional quantum materials that remain strongly ferromagnetic down to mono layer thickness are highly desired for spintronic applications. Although oxide materials are important candidates for next generation of spintronic, ferromagnetism decays severely when the thickness is scaled to the nano meter regime, leading to deterioration of device performance. Here we report a methodology for maintaining strong ferromagnetism in insulating LaCoO3 (LCO) layers down to the thickness of a single unit cell. We find that the magnetic and electronic states of LCO are linked intimately to the structural parameters of adjacent "breathing lattice" SrCuO2 (SCO). As the dimensionality of SCO is reduced, the lattice constant elongates over 10% along the growth direction, leading to a significant distortion of the CoO6 octahedra, and promoting a higher spin state and long-range spin ordering. For atomically thin LCO layers, we observe surprisingly large magnetic moment (0.5 uB/Co) and Curie temperature (75 K), values larger than previously reported for any mono layer oxide. Our results demonstrate a strategy for creating ultra thin ferromagnetic oxides by exploiting atomic hetero interface engineering,confinement-driven structural transformation, and spin-lattice entanglement in strongly correlated materials., Comment: 24 pages, 5 figures, 1 supporting information with 13 figures

Strain engineering provides the ability to control the ground states and associated phase transition in the epitaxial films. However, the systematic study of intrinsic characters and their strain dependency in transition-metal nitrides remains challenging due to the difficulty in fabricating the stoichiometric and high-quality films. Here we report the observation of electronic state transition in highly crystalline antiferromagnetic CrN films with strain and reduced dimensionality. Shrinking the film thickness to a critical value of ~ 30 unit cells, a profound conductivity reduction accompanied by unexpected volume expansion is observed in CrN films. The electrical conductivity is observed surprisingly when the CrN layer as thin as single unit cell thick, which is far below the critical thickness of most metallic films. We found that the metallicity of an ultrathin CrN film recovers from an insulating behavior upon the removal of as-grown strain by fabrication of first-ever freestanding nitride films. Both first-principles calculations and linear dichroism measurements reveal that the strain-mediated orbital splitting effectively customizes the relatively small bandgap at the Fermi level, leading to exotic phase transition in CrN. The ability to achieve highly conductive nitride ultrathin films by harness strain-controlling over competing phases can be used for utilizing their exceptional characteristics., Comment: 24 pages, 5 figures

Polar metals with ferroelectric-like displacements in metals have been achieved recently, half century later than Anderson and Blount's prediction. However, the genuine ferroelectricity with electrical dipolar switching has not yet been attained experimentally in the conducting materials, especially the ones possessing magnetic responses. Here we report the coexistence of ferroelectricity and magnetoresistance (MR) in the metallic PbNb0.12Ti0.88O3 (PNTO) thin films. We found that the conducting and magnetic responses of PNTO films are highly asymmetric. Negative MR up to 50% is observed under an in-plane magnetic field; the MR switches to positive with the magnetic field applied parallel to the surface normal. Such unique behavior is attributed to the moving electron caused effective magnetic field which couples with the spins of electrons, which form a dynamic multiferroic state in the metallic PNTO. These findings break a path to multiferroic metal and offer a great potential to the multi-functional devices., Comment: 21 pages, 3 figures

Despite of the tremendous efforts spent on the oxygen vacancy migration in determining the property optimization of oxygen-vacancy enrichment transition metal oxides, few has focused on their dynamic behaviors non-equilibrium states. In this work, we performed multi-timescale ultrafast X-ray diffraction measurements by using picosecond synchrotron X-ray pulses and femtosecond table-top X-ray pulses to monitor the structural dynamics in the oxygen-vacancy ordered SrCoO2.5 thin films. A giant photoinduced strain ({\Delta}c/c > 1%) was observed, whose distinct correlation with the pump photon energy indicates a non-thermal origin of the photoinduced strain. The sub-picosecond resolution X-ray diffraction reveals the formation and propagation of the coherent acoustic phonons inside the film. We also simulate the effect of photoexcited electron-hole pairs and the resulting lattice changes using the Density Function Theory method to obtain further insight on the microscopic mechanism of the measured photostriction effect. Comparable photostrictive responses and the strong dependence on excitation wavelength are predicted, revealing a bonding to anti-bonding charge transfer or high spin to intermediate spin crossover induced lattice expansion in the oxygen-vacancy films., Comment: 12 pages, 4 figures, support material