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Register a new userCompressive-strain induced enhancement of exchange interactions and short-range magnetic order in Sr$_2$IrO$_4$ investigated by Raman spectroscopy
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We have carried out Raman spectroscopy experiments to investigate two-magnon excitations in epitaxial thin films of the quasi-two-dimensional antiferromagnetic Mott insulator Sr$_2$IrO$_4$ under in-plane misfit strain. With in-plane biaxial compression, the energy of the two-magnon peak increases, and the peak remains observable over a wider temperature range above the Neel temperature, indicating strain-induced enhancement of the superexchange interactions between $it{J}_{eff}$ = 1/2 pseudospins. From density functional theory calculations, we have found an increase of the nearest-neighbor hopping parameter and exchange interaction with increasing biaxial compressive strain, in agreement with the experimental observations. Our experimental and theoretical results provide perspectives for systematic, theory-guided strain control of the primary exchange interactions in 5$it{d}$ transition metal oxides.
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We report a La2CuO4-like interlayer antiferromagnetic order in Sr2IrO4 films with large orthorhombic distortion (> 1.5%). The biaxial lattice strain in epitaxial heterostructures of Sr2IrO4/Ca3Ru2O7 lowers the crystal symmetry of Sr2IrO4 from tetragonal (C4) to orthorhombic (C2), guiding the Ir 5d Jeff = 1/2 pseudospin moment parallel to the elongated b-axis via magnetic anisotropy. From resonant X-ray scattering experiments, we observed an antiferromagnetic order in the orthorhombic Sr2IrO4 film whose interlayer stacking pattern is inverted from that of the tetragonal Sr2IrO4 crystal. This interlayer stacking is similar to that of the orthorhombic La2CuO4, implying that the asymmetric interlayer exchange interaction along a and b-directions exceeds the anisotropic interlayer pseudo-dipolar interaction. Our result suggests that strain-induced distortion can provide a delicate knob for tuning the long-range magnetic order in quasi-two-dimensional systems by evoking the competition between the interlayer exchange coupling and the pseudo-dipolar interaction.
We investigate the crystal structure and lattice vibrations of Sr$_2$IrO$_4$ by a combined phonon Raman scattering and x-ray powder diffraction experiment under pressures up to $66$ GPa and room temperature. Density functional theory (DFT) and $ab$-initio lattice dynamics calculations were also carried out. A first-order structural phase transition associated with an $8$ % collapse of the $c$-axis is observed at high pressures, with phase coexistence being observed between $sim 40$ and $55$ GPa. At lower pressures, lattice and phonon anomalies were observed, reflecting crossovers between isostructural competing states. A critical pressure of $P_1=17$ GPa is associated with: (i) a reduction of lattice volume compressibility and a change of behavior of the tetragonal $c/a$ ratio take place above $P_1$; (ii) a four-fold symmetry-breaking lattice strain associated with lattice disorder; (iii) disappearance of two Raman active modes (at $sim 180$ and $sim 260$ cm$^{-1}$); and (iv) development of an asymmetric Fano lineshape for the $sim 390$ cm$^{-1}$ mode. DFT indicates that the phase above $P_1$ is most likely non-magnetic. Exploring the similarities between iridate and cuprate physics, we argue that these observations are consistent with the emergence of a rotational symmetry-breaking electronic instability at $P_1$, providing hints for the avoided metallization under pressure and supporting the hypothesis of possible competing orders that are detrimental to superconductivity in this family. Alternative scenarios for the transition at $P_1$ are also suggested and critically discussed. Additional phonon and lattice anomalies in the tetragonal phase are observed at $P_2=30$ and $P_3=40$ GPa, indicating further competing phases that are stabilized at high pressures.
We show that, contrary to previous belief, the transition to the antiferromagnetic state of Sr$_2$IrO$_4$ in zero magnetic field does show up in the transverse resistivity. We attribute this to a change in transverse integrals associated to the magnetic ordering, which is evaluated considering hopping of the localized charge. The evolution of the resistivity anomaly associated to the magnetic transition under applied magnetic field is studied. It tracks the magnetic phase diagram, allowing to identify three different lines, notably the spin-flip line, associated with the reordering of the ferromagnetic component of the magnetization, and an intriguing line for field induced magnetism, also corroborated by magnetization measurements.
We report the existence of Griffiths phase (GP) and its influence on critical phenomena in layered Sr$_2$IrO$_4$ ferromagnet (T$_C$ = 221.5 K). The power law behavior of inverse magentic susceptibility, 1/$chi$(T) with exponent $lambda = 0.18(2)$ confirm the GP in the regime T$_C$ $<$ T $leq$ T$_G$ = 279.0(5) K. Moreover, the detailed critical analysis via modified Arrott plot method exhibits unrealistic critical exponents $beta$ = 0.77(1), $gamma$ = 1.59(2) and $delta = 3.06(4)$, in corroboration with magneto-caloric study. The abnormal exponent values have been viewed in context of ferromagnetic-Griffiths phase transition. The GP has been further analyzed using Bray model, which yields a reliable value of $beta$ = 0.19(2), belonging to the two-dimensional (2D) XYh$_4$ universality class with strong anisotropy present in Sr$_2$IrO$_4$. The present study proposes Bray model as a possible tool to investigate the critical behavior for Griffiths ferromagnets in place of conventional Arrott plot analysis. The possible origins of GP and its correlation with insulating nature of Sr$_2$IrO$_4$ have been discussed.
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.
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