skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Atomic order of rare earth ions in a complex oxide: a path to magnetotaxial anisotropy
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
Award ID(s):
2323132 1808190 2232830
PAR ID:
10514837
Author(s) / Creator(s):
; ; ; ; ; ; ; ;
Publisher / Repository:
Nature Publishing Group
Date Published:
Journal Name:
Nature Communications
Volume:
15
Issue:
1
ISSN:
2041-1723
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract Rare‐earth iron garnets (REIG) have recently become the materials platform of choice for spintronic studies on ferrimagnetic insulators. However, thus far the materials studied have mainly been REIG with a single rare earth species such as thulium, yttrium, or terbium iron garnets. In this study, magnetometry, ferromagnetic resonance, and magneto‐optical Kerr effect imaging is used to explore the continuous variation of magnetic properties as a function of composition for YxTm3−xiron garnet (YxTm3−xIG) thin films grown by pulsed laser deposition on gadolinium gallium garnet substrates. It is reported that the tunability of the magnetic anisotropy energy, with full control achieved over the type of anisotropy (from perpendicular, to isotropic, to an in‐plane easy axis) on the same substrate. In addition, a nonmonotonic composition‐dependent anisotropy term is reported, which is ascribed to growth‐induced anisotropy similar to what is reported in garnet thin films grown by liquid‐phase epitaxy. Ferromagnetic resonance shows linear variation of the damping and the g‐factor across the composition range, consistent with prior theoretical work. Domain imaging reveals differences in reversal modes, remanant states, and domain sizes in YxTm3−xiron‐garnet thin films as a function of anisotropy. 
    more » « less
  2. Abstract Complex oxide films stabilized by epitaxial growth can exhibit large populations of point defects which have important effects on their properties. The site occupancy of pulsed laser‐deposited epitaxial terbium iron garnet (TbIG) films with excess terbium (Tb) is analyzed, in which the terbium:iron (Tb:Fe)ratio is 0.86 compared to the stoichiometric value of 0.6. The magnetic properties of the TbIG are sensitive to site occupancy, exhibiting a higher compensation temperature (by 90 K) and a lower Curie temperature (by 40 K) than the bulk Tb3Fe5O12garnet. Data derived from X‐ray core‐level spectroscopy, magnetometry, and molecular field coefficient modeling are consistent with occupancy of the dodecahedral sites by Tb3+, the octahedral sites by Fe3+, Tb3+and vacancies, and the tetrahedral sites by Fe3+and vacancies. Energy dispersive X‐ray spectroscopy in a scanning transmission electron microscope provides direct evidence of TbFeantisites. A small fraction of Fe2+is present, and oxygen vacancies are inferred to be present to maintain charge neutrality. Variation of the site occupancies provides a path to considerable manipulation of the magnetic properties of epitaxial iron garnet films and other complex oxides, which readily accommodate stoichiometries not found in their bulk counterparts. 
    more » « less
  3. Abstract One of the best magneto‐optical claddings for optical isolators in photonic integrated circuits is sputter deposited cerium‐doped terbium iron garnet (Ce:TbIG) which has a large Faraday rotation (≈−3500° cm−1at 1550 nm). Near‐ideal stoichiometry of Ce0.5Tb2.5Fe4.75O12is found to have a 44 nm magnetic dead layer that can impede the interaction of propagating modes with garnet claddings. The effective anisotropy of Ce:TbIG on Si is also important, but calculations using bulk thermal mismatch overestimate the effective anisotropy. Here, X‐ray diffraction measurements yield highly accurate measurements of strain that show anisotropy favors an in‐plane magnetization in agreement with the positive magnetostriction of Ce:TbIG. Upon doping TbIG with Ce, a slight decrease in compensation temperature occurs which points to preferential rare‐earth occupation in dodecahedral sites and an absence of cation redistribution between different lattice sites. The high Faraday rotation, large remanent ratio, large coercivity, and preferential in‐plane magnetization enable Ce:TbIG to be an in‐plane latched garnet, immune to stray fields with magnetization collinear to direction of light propagation. 
    more » « less
  4. Abstract Single-phase multiferroic materials that allow the coexistence of ferroelectric and magnetic ordering above room temperature are highly desirable, motivating an ongoing search for mechanisms for unconventional ferroelectricity in magnetic oxides. Here, we report an antisite defect mechanism for room temperature ferroelectricity in epitaxial thin films of yttrium orthoferrite, YFeO 3 , a perovskite-structured canted antiferromagnet. A combination of piezoresponse force microscopy, atomically resolved elemental mapping with aberration corrected scanning transmission electron microscopy and density functional theory calculations reveals that the presence of Y Fe antisite defects facilitates a non-centrosymmetric distortion promoting ferroelectricity. This mechanism is predicted to work analogously for other rare earth orthoferrites, with a dependence of the polarization on the radius of the rare earth cation. Our work uncovers the distinctive role of antisite defects in providing a mechanism for ferroelectricity in a range of magnetic orthoferrites and further augments the functionality of this family of complex oxides for multiferroic applications. 
    more » « less
  5. Abstract The vast high entropy alloy (HEA) composition space is promising for discovery of new material phases with unique properties. This study explores the potential to achieve rare‐earth‐free high magnetic anisotropy materials in single‐phase HEA thin films. Thin films of FeCoNiMnCu sputtered on thermally oxidized Si/SiO2substrates at room temperature are magnetically soft, with a coercivity on the order of 10 Oe. After post‐deposition rapid thermal annealing (RTA), the films exhibit a single face‐centered‐cubic phase, with an almost 40‐fold increase in coercivity. Inclusion of 50 at.% Pt in the film leads to ordering of a singleL10high entropy intermetallic phase after RTA, along with high magnetic anisotropy and 3 orders of magnitude coercivity increase. These results demonstrate a promising HEA approach to achieve high magnetic anisotropy materials using RTA. 
    more » « less