skip to main content


Title: Emergent long-range magnetic order in ultrathin (111)-oriented LaNiO3 films
Abstract

The emergence of ferromagnetism in materials where the bulk phase does not show any magnetic order demonstrates that atomically precise films can stabilize distinct ground states and expands the phase space for the discovery of materials. Here, the emergence of long-range magnetic order is reported in ultrathin (111) LaNiO3(LNO) films, where bulk LNO is paramagnetic, and the origins of this phase are explained. Transport and structural studies of LNO(111) films indicate that NiO6octahedral distortions stabilize a magnetic insulating phase at the film/substrate interface and result in a thickness-dependent metal–insulator transition att = 8 unit cells. Away from this interface, distortions relax and bulk-like conduction is regained. Synchrotron x-ray diffraction and dynamical x-ray diffraction simulations confirm a corresponding out-of-plane unit-cell expansion at the interface of all films. X-ray absorption spectroscopy reveals that distortion stabilizes an increased concentration of Ni2+ions. Evidence of long-range magnetic order is found in anomalous Hall effect and magnetoresistance measurements, likely due to ferromagnetic superexchange interactions among Ni2+–Ni3+ions. Together, these results indicate that long-range magnetic ordering and metallicity in LNO(111) films emerges from a balance among the spin, charge, lattice, and orbital degrees of freedom.

 
more » « less
PAR ID:
10227677
Author(s) / Creator(s):
; ; ; ; ; ; ; ;
Publisher / Repository:
Nature Publishing Group
Date Published:
Journal Name:
npj Quantum Materials
Volume:
6
Issue:
1
ISSN:
2397-4648
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. The temperature-dependent layer-resolved structure of 3 to 44 unit cell thick SrRuO 3 (SRO) films grown on Nb-doped SrTiO 3 substrates is investigated using a combination of high-resolution synchrotron x-ray diffraction and high-resolution electron microscopy to understand the role that structural distortions play in suppressing ferromagnetism in ultra-thin SRO films. The oxygen octahedral tilts and rotations and Sr displacements characteristic of the bulk orthorhombic phase are found to be strongly dependent on temperature, the film thickness, and the distance away from the film–substrate interface. For thicknesses, t, above the critical thickness for ferromagnetism ( t > 3 uc), the orthorhombic distortions decrease with increasing temperature above T C . Below T C , the structure of the films remains constant due to the magneto-structural coupling observed in bulk SRO. The orthorhombic distortions are found to be suppressed in the 2–3 interfacial layers due to structural coupling with the SrTiO 3 substrate and correlate with the critical thickness for ferromagnetism in uncapped SRO films. 
    more » « less
  2. Abstract

    Complex oxides offer rich magnetic and electronic behavior intimately tied to the composition and arrangement of cations within the structure. Rare earth iron garnet films exhibit an anisotropy along the growth direction which has long been theorized to originate from the ordering of different cations on the same crystallographic site. Here, we directly demonstrate the three-dimensional ordering of rare earth ions in pulsed laser deposited (EuxTm1-x)3Fe5O12garnet thin films using both atomically-resolved elemental mapping to visualize cation ordering and X-ray diffraction to detect the resulting order superlattice reflection. We quantify the resulting ordering-induced ‘magnetotaxial’ anisotropy as a function of Eu:Tm ratio using transport measurements, showing an overwhelmingly dominant contribution from magnetotaxial anisotropy that reaches 30 kJ m−3for garnets with x = 0.5. Control of cation ordering on inequivalent sites provides a strategy to control matter on the atomic level and to engineer the magnetic properties of complex oxides.

     
    more » « less
  3. Abstract

    We report on the structure and dielectric properties of ternary A6B2O17(A = Zr; B = Nb, Ta) thin films and ceramics. Thin films are produced via sputter deposition from dense, phase‐homogenous bulk ceramic targets, which are synthesized through a reactive sintering process at 1500°C. Crystal structure, microstructure, chemistry, and dielectric properties are characterized by X‐ray diffraction and reflectivity, atomic force microscopy, X‐ray photoelectron spectroscopy, and capacitance analysis, respectively. We observe relative permittivities approaching 60 and loss tangents <1 × 10−2across the 103–105 Hz frequency range in the Zr6Nb2O17and Zr6Ta2O17phases. These observations create an opportunity space for this novel class of disordered oxide electroceramics.

     
    more » « less
  4. Abstract

    Intrinsic exchange bias is known as the unidirectional exchange anisotropy that emerges in a nominally single-component ferro-(ferri-)magnetic system. In this work, with magnetic and structural characterizations, we demonstrate that intrinsic exchange bias is a general phenomenon in (Ni, Co, Fe)-based spinel oxide films deposited onα-Al2O3(0001) substrates, due to the emergence of a rock-salt interfacial layer consisting of antiferromagnetic CoO from interfacial reconstruction. We show that in NixCoyFe3−xyO4(111)/α-Al2O3(0001) films, intrinsic exchange bias and interfacial reconstruction have consistent dependences on Co concentrationy, while the Ni and Fe concentration appears to be less important. This work establishes a family of intrinsic exchange bias materials with great tunability by stoichiometry and highlights the strategy of interface engineering in controlling material functionalities.

     
    more » « less
  5. Neutron powder diffraction (NPD) and x-ray magnetic circular dichroism (XMCD) spectroscopy are employed to investigate the magnetism and spin structure in single-phase B20 Co1.043Si0.957. The magnetic contributions to the NPD data measured in zero fields are consistent with the helical order among the allowed spin structures derived from group theory. The magnitude of the magnetic moment is (0.3 ± 0.1) μB/Co according to NPD, while the surface magnetization probed by XMCD at 3 kOe is (0.18–0.31) μB/Co. Both values are substantially larger than the bulk magnetization of 0.11 μB/Co determined from magnetometry at 70 kOe and 2 K. These experimental data indicate the formation of a helical spin phase and the associated conical states in high magnetic fields.

     
    more » « less