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Register a new userGiant Magneto-electric Effect in the Novel Mott Insulator, Sr2IrO4
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Our magnetic, electrical, and thermal measurements on single-crystals of the novel Mott insulator, Sr2IrO4, reveal a novel giant magneto-electric effect (GME) arising from a frustrated magnetic/ferroelectric state whose signatures are: (1) a strongly enhanced electric permittivity that peaks near a newly observed magnetic anomaly at 100 K, (2) a large (~100%) magneto-dielectric shift that occurs near a metamagnetic transition, and (3) magnetic and electric polarization hysteresis. The GME and electric polarization hinge on a spin-orbit gapping of 5d-bands, rather than the magnitude and spatial dependence of magnetization, as traditionally accepted.
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Spin-orbit entangled magnetic dipoles, often referred to as pseudospins, provide a new avenue to explore novel magnetism inconceivable in the weak spin-orbit coupling limit, but the nature of their low-energy interactions remains to be understood. We present a comprehensive study of the static magnetism and low-energy pseudospin dynamics in the archetypal spin-orbit Mott insulator Sr2IrO4. We find that in order to understand even basic magnetization measurements, a formerly overlooked in-plane anisotropy is fundamental. In addition to magnetometry, we use neutron diffraction, inelastic neutron scattering and resonant elastic and inelastic x-ray scattering to identify and quantify the interactions that determine the global symmetry of the system and govern the linear responses of pseudospins to external magnetic felds and their low-energy dynamics. We find that a pseudospin-only Hamiltonian is insufficient for an accurate description of the magnetism in Sr2IrO4 and that pseudospin-lattice coupling is essential. This finding should be generally applicable to other pseudospin systems with sizable orbital moments sensitive to anisotropic crystalline environments.
X-ray absorption near edge spectra (XANES) and magnetization of Zn doped MnV2O4 have been measured and from the magnetic measurement the critical exponents and magnetocaloric effect have been estimated. The XANES study indicates that Zn doping does not change the valence states in Mn and V. It has been shown that the obtained values of critical exponents b{eta}, {gamma} and {delta} do not belong to universal class and the values are in between the 3D Heisenberg model and the mean field interaction model. The magnetization data follow the scaling equation and collapse into two branches indicating that the calculated critical exponents and critical temperature are unambiguous and intrinsic to the system. All the samples show large magneto-caloric effect. The second peak in magneto-caloric curve of Mn0.95Zn0.05V2O4 is due to the strong coupling between orbital and spin degrees of freedom. But 10% Zn doping reduces the residual spins on the V-V pairs resulting the decrease of coupling between orbital and spin degrees of freedom.
We investigated electronic structure of 5d transition-metal oxide Sr2IrO4 using angle-resolved photoemission, optical conductivity, and x-ray absorption measurements and first-principles band calculations. The system was found to be well described by novel effective total angular momentum Jeff states, in which relativistic spin-orbit (SO) coupling is fully taken into account under a large crystal field. Despite of delocalized Ir 5d states, the Jeff-states form so narrow bands that even a small correlation energy leads to the Jeff = 1/2 Mott ground state with unique electronic and magnetic behaviors, suggesting a new class of the Jeff quantum spin driven correlated-electron phenomena.
In Mott insulators, the strong electron-electron Coulomb repulsion prevents metallicity and charge excitations are gapped. In dimensions greater than one, their spins are usually ordered antiferromagnetically at low temperatures. Geometrical frustrations can destroy this long-range order, leading to exotic quantum spin liquid (QSL) states. However, their magnetic ground states have been a long-standing mystery. Here we show that a QSL state in the organic Mott insulator EtMe$_3$Sb[Pd(dmit)$_2$]$_2$ with two-dimensional triangular lattice has Pauli-paramagnetic-like low-energy excitations, which are a hallmark of itinerant fermions. Our torque magnetometry down to low temperatures (30 mK) up to high fields (32 T) reveal distinct residual paramagnetic susceptibility comparable to that in a half-filled two-dimensional metal. This demonstrates that the system is in a magnetically gapless ground state, a critical state with infinite magnetic correlation length. Moreover, our results are robust against deuteration, pointing toward the emergence of an extended `quantum critical phase, in which low-energy spin excitations behave as in paramagnetic metals with Fermi surface, despite the frozen charge degree of freedom.
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.
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