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.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


  • NSF Public Access
  • Search Results
  • Imaging antiferromagnetic domain fluctuations and the effect of atomic scale disorder in a doped spin-orbit Mott insulator
Title: Imaging antiferromagnetic domain fluctuations and the effect of atomic scale disorder in a doped spin-orbit Mott insulator
Correlated oxides can exhibit complex magnetic patterns. Understanding how magnetic domains form in the presence of disorder and their robustness to temperature variations has been of particular interest, but atomic scale insight has been limited. We use spin-polarized scanning tunneling microscopy to image the evolution of spin-resolved modulations originating from antiferromagnetic (AF) ordering in a spin-orbit Mott insulator perovskite iridate Sr 3 Ir 2 O 7 as a function of chemical composition and temperature. We find that replacing only several percent of lanthanum for strontium leaves behind nanometer-scale AF puddles clustering away from lanthanum substitutions preferentially located in the middle strontium oxide layer. Thermal erasure and reentry into the low-temperature ground state leads to a spatial reorganization of the AF puddles, which nevertheless maintain scale-invariant fractal geometry in each configuration. Our experiments reveal multiple stable AF configurations at low temperature and shed light onto spatial fluctuations of the AF order around atomic scale disorder in electron-doped Sr 3 Ir 2 O 7 .  more » « less
Award ID(s):
1905801
PAR ID:
10346512
Author(s) / Creator(s):
; ; ; ; ;
Date Published:
Journal Name:
Science Advances
Volume:
7
Issue:
46
ISSN:
2375-2548
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; ; ; ; ; ; ; ; et al (, Journal of Physics: Condensed Matter)
    Abstract With the motivation to study how non-magnetic ion site disorder affects the quantum magnetism of Ba 3 CoSb 2 O 9 , a spin-1/2 equilateral triangular lattice antiferromagnet, we performed DC and AC susceptibility, specific heat, elastic and inelastic neutron scattering measurements on single crystalline samples of Ba 2.87 Sr 0.13 CoSb 2 O 9 with Sr doping on non-magnetic Ba 2+ ion sites. The results show that Ba 2.87 Sr 0.13 CoSb 2 O 9 exhibits (i) a two-step magnetic transition at 2.7 K and 3.3 K, respectively; (ii) a possible canted 120 degree spin structure at zero field with reduced ordered moment as 1.24 μ B /Co; (iii) a series of spin state transitions for both H ∥ ab -plane and H ∥ c -axis. For H ∥ ab -plane, the magnetization plateau feature related to the up–up–down phase is significantly suppressed; (iv) an inelastic neutron scattering spectrum with only one gapped mode at zero field, which splits to one gapless and one gapped mode at 9 T. All these features are distinctly different from those observed for the parent compound Ba 3 CoSb 2 O 9 , which demonstrates that the non-magnetic ion site disorder (the Sr doping) plays a complex role on the magnetic properties beyond the conventionally expected randomization of the exchange interactions. We propose the additional effects including the enhancement of quantum spin fluctuations and introduction of a possible spatial anisotropy through the local structural distortions. 
    more » « less
  2. ; ; ; ; ; ; ; ; (, Journal of Physics: Condensed Matter)
    Abstract We report evidence of a finite density of states at the Fermi level at the surface of epitaxial thin films of the narrow bandgap Mott insulator Sr3Ir2O7(001). The Brillouin zone critical points for Sr3Ir2O7(001) thin films have been determined by a comparison of the band mapping from angle-resolved photoemission spectroscopy and low energy electron diffraction. Angle-resolved x-ray photoemission studies reveal the surface termination of Sr3Ir2O7(001) is Sr–O. The absence of dispersion with photon energy, or changing wave vector along the surface normal, indicates the two-dimensional character of the bands contributing to the density of states close to the Fermi level for Sr3Ir2O7(001) thin films. Thus, the finite density of states at the Fermi level is attributed to surface states or surface resonances. The appearance of a finite density of states at the Fermi level is consistent with the increased conductivity with decreasing film thickness for ultrathin Sr3Ir2O7(001) films. 
    more » « less
  3. ; ; ; ; ; ; ; ; ; ; et al (, Nature Communications)
    Abstract Excitonic insulators are usually considered to form via the condensation of a soft charge mode of bound electron-hole pairs. This, however, presumes that the soft exciton is of spin-singlet character. Early theoretical considerations have also predicted a very distinct scenario, in which the condensation of magnetic excitons results in an antiferromagnetic excitonic insulator state. Here we report resonant inelastic x-ray scattering (RIXS) measurements of Sr 3 Ir 2 O 7 . By isolating the longitudinal component of the spectra, we identify a magnetic mode that is well-defined at the magnetic and structural Brillouin zone centers, but which merges with the electronic continuum in between these high symmetry points and which decays upon heating concurrent with a decrease in the material’s resistivity. We show that a bilayer Hubbard model, in which electron-hole pairs are bound by exchange interactions, consistently explains all the electronic and magnetic properties of Sr 3 Ir 2 O 7 indicating that this material is a realization of the long-predicted antiferromagnetic excitonic insulator phase. 
    more » « less
  4. ; ; ; ; ; ; (, Journal of Materials Chemistry A)
    The significant role of perovskite defect chemistry through A-site doping of strontium titanate with lanthanum for CO 2 electrolysis properties is demonstrated. Here we present a dual strategy of A-site deficiency and promoting adsorption/activation by making use of redox active dopants such as Mn/Cr linked to oxygen vacancies to facilitate CO 2 reduction at perovskite titanate cathode surfaces. Solid oxide electrolysers based on oxygen-excess La 0.2 Sr 0.8 Ti 0.9 Mn(Cr) 0.1 O 3+δ , A-site deficient (La 0.2 Sr 0.8 ) 0.9 Ti 0.9 Mn(Cr) 0.1 O 3−δ and undoped La 0.2 Sr 0.8 Ti 1.0 O 3+δ cathodes are evaluated. In situ infrared spectroscopy reveals that the adsorbed and activated CO 2 adopts an intermediate chemical state between a carbon dioxide molecule and a carbonate ion. The double strategy leads to optimal performance being observed after 100 h of high-temperature operation and 3 redox cycles, suggesting a promising cathode material for CO 2 electrolysis. 
    more » « less
  5. ; ; ; ; ; (, Journal of Physics: Condensed Matter)
    Abstract We report on the temperature dependent low energy electron diffraction (LEED) studies of 12 nm epitaxial Sr3Ir2O7(001) thin films. The Debye temperature has been extracted from the temperature-dependence of LEED intensity at elevated temperatures and different electron kinetic energies. For the most surface sensitive LEED, obtained at the lowest electron kinetic energies, the extracted surface Debye temperature is 270 ± 22 K, which is much lower than the 488 ± 40 K Debye temperature obtained using higher electron kinetic energies. Surprisingly, the LEED diffraction intensity, at the lowest electron kinetic energies, increases rather than decreases, with increasing sample temperatures up to about 440 K. This anomalous behavior has been attributed to the reduction of the lattice vibrational amplitudes along the surface normal. This damping of the normal mode vibrations with increasing temperature results from the enhanced electronic screening via thermally activated carriers. This scenario is corroborated by the transport measurement, showing that Sr3Ir2O7is a narrow band Mott insulator with a band gap of about 32 meV. We have identified criteria for finding anomalous scattering behavior in other transition metal oxide systems. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Text Encoded Conversion
  • XML
  • Save / Share this Record
  • Send to Email