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Precise control of $J_mathrm{eff}=1/2$ magnetic properties in Sr$_2$IrO$_4$ epitaxial thin films by variation of strain and thin film thickness

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 Added by Stephan Gepr\\\"ags
 Publication date 2020
  fields Physics
and research's language is English




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We report on a comprehensive investigation of the effects of strain and film thickness on the structural and magnetic properties of epitaxial thin films of the prototypal $J_mathrm{eff}=1/2$ compound Sr$_2$IrO$_4$ by advanced X-ray scattering. We find that the Sr$_2$IrO$_4$ thin films can be grown fully strained up to a thickness of 108 nm. By using X-ray resonant scattering, we show that the out-of-plane magnetic correlation length is strongly dependent on the thin film thickness, but independent of the strain state of the thin films. This can be used as a finely tuned dial to adjust the out-of-plane magnetic correlation length and transform the magnetic anisotropy from two-dimensional (2D) to three-dimensional (3D) behavior by incrementing film thickness. These results provide a clearer picture for the systematic control of the magnetic degrees of freedom in epitaxial thin films of Sr$_2$IrO$_4$ and bring to light the potential for a rich playground to explore the physics of $5d$-transition metal compounds.



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Thin films of the ferromagnetic metal SrRuO3 (SRO) show a varying easy magnetization axis depending on the epitaxial strain and undergo a metal-to-insulator transition with decreasing film thickness. We have investigated the magnetic properties of SRO thin films with varying thicknesses fabricated on SrTiO3(001) substrates by soft x-ray magnetic circular dichroism (XMCD) at the Ru M2,3 edge. Results have shown that, with decreasing film thickness, the film changes from ferromagnetic to non-magnetic around 3monolayer thickness, consistent with previous magnetization and magneto-optical Kerr effect measurements. The orbital magnetic moment perpendicular to the film was found to be ~ 0.1{mu}B/Ru atom, and remained nearly unchanged with decreasing film thickness while the spin magnetic moment decreases. Mechanism for the formation of the orbital magnetic moment is discussed based on the electronic structure of the compressively strained SRO film.
$5d$ iridium oxides are of huge interest due to the potential for new quantum states driven by strong spin-orbit coupling. The strontium iridate Sr$_2$IrO$_4$ is particularly in the spotlight because of the so-called $j_text{eff}=1/2$ state consisting of a quantum superposition of the three local $t_{2g}$ orbitals with -- in its most simple version -- nearly equal population, which stabilizes an unconventional Mott insulating state. Here, we report an anisotropic and aspherical magnetization density distribution measured by polarized neutron diffraction in a magnetic field up to 5~T at 4~K, which strongly deviates from a local jeffHalf picture even when distortion-induced deviations from the equal weights of the orbital populations are taken into account. Once reconstructed by the maximum entropy method and multipole expansion model refinement, the magnetization density shows cross-shaped positive four lobes along the crystallographic tetragonal axes with a large spatial extent, showing that the $xy$ orbital contribution is dominant. The analogy to the superconducting copper oxide systems might then be weaker than commonly thought.
Motivated by the success of experimental manipulation of the band structure through biaxial strain in Sr$_2$RuO$_4$ thin film grown on a mismatched substrate, we investigate theoretically the effects of biaxial strain on the electronic instabilities, such as superconductivity (SC) and spin density wave (SDW), by functional renormalization group. According to the experiment, the positive strain (from lattice expansion) causes charge transfer to the $gamma$-band and consequently Lifshitz reconstruction of the Fermi surface. Our theoretical calculations show that within a limited range of positive strain a p-wave superconducting order is realized. However, as the strain is increased further the system develops into the SDW state well before the Lifshitz transition is reached. We also consider the effect of negative strains (from lattice constriction). As the strain increases, there is a transition from p-wave SC state to nodal s-wave SC state. The theoretical results are discussed in comparison to experiment and can be checked by further experiments.
The anisotropic magnetic properties of Sr$_2$IrO$_4$ are investigated, using longitudinal and torque magnetometry. The critical scaling across $T_c$ of the longitudinal magnetization is the one expected for the 2D XY universality class. Modeling the torque for a magnetic field in the basal-plane, and taking into account all in-plane and out-of-plane magnetic couplings, we derive the effective 4-fold anisotropy $K_4 approx$ 1 10$^5$ erg mole$^{-1}$. Although larger than for the cuprates, it is found too small to account for a significant departure from the isotropic 2D XY model. The in-plane torque also allows us to put an upper bound for the anisotropy of a field-induced shift of the antiferromagnetic ordering temperature.
A structural transition in an ABO$_{3}$ perovskite thin film involving the change of the BO$_{6}$ octahedral rotation pattern can be hidden under the global lattice symmetry imposed by the substrate and often easily overlooked. We carried out high-resolution x-ray diffraction experiments to investigate the structures of epitaxial Ca$_{0.5}$Sr$_{0.5}$IrO$_{3}$ (CSIO) perovskite iridate films grown on the SrTiO$_{3}$ (STO) and GdScO$_{3}$ (GSO) substrates in detail. Although the CSIO/STO film layer displays a global tetragonal lattice symmetry evidenced by the reciprocal space mapping, synchrotron x-ray data indicates that its room temperature structure is monoclinic due to Glazers a$^{+}$a$^{-}$c$^{-}$-type rotation of the IrO$_{6}$ octahedra. In order to accommodate the lower-symmetry structure under the global tetragonal symmetry, the film breaks into four twinned domains, resulting in the splitting of the (half-integer, 0, integer) superlattice reflections. Surprisingly, the splitting of these superlattice reflections decrease with increasing temperature, eventually disappearing at T$_{S}$ = 510(5) K, which signals a structural transition to an orthorhombic phase with a$^{+}$a$^{-}$c$^{0}$ octahedral rotation. In contrast, the CSIO/GSO film displays a stable monoclinic symmetry with a$^{+}$b$^{-}$c$^{-}$ octahedral rotation, showing no structural instability caused by the substrate up to 520 K. Our study illustrates the importance of the symmetry in addition to the lattice mismatch of the substrate in determining the structure of epitaxial thin films.
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