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Leveraging coherent light-matter interaction in solids is a promising new direction towards control and functionalization of quantum materials, to potentially realize regimes inaccessible in equilibrium and stabilize new or useful states of matter. We show how driving the strongly spin-orbit coupled proximal Kitaev magnet $alpha$-RuCl$_3$ with circularly-polarized light can give rise to a novel ligand-mediated magneto-electric effect that both photo-induces a large dynamical effective magnetic field and dramatically alters the interplay of competing isotropic and anisotropic exchange interactions. We propose that tailored light pulses can nudge the material towards the elusive Kitaev quantum spin liquid as well as probe competing magnetic instabilities far from equilibrium, and predict that the transient competition of magnetic exchange processes can be readily observed via pump-probe spectroscopy.
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Recent discovery of the half quantized thermal Hall conductivity in $alpha$-RuCl$_3$, a candidate material for the Kitaev spin liquid, suggests the presence of a highly entangled quantum state in external magnetic fields. This field induced phase appears between the low field zig-zag magnetic order and the high field polarized state. Motivated by this experiment, we study possible field induced quantum phases in theoretical models of the Kitaev magnets, using the two dimensional tensor network approach or infinite tensor product states. We find various quantum ground states in addition to the chiral Kitaev spin liquid occupying a small area in the phase diagram. They form a band of emergent quantum phases in an intermediate window of external magnetic fields, somewhat reminiscent of the experiment. We discuss the implications of these results in view of the experiment and previous theoretical studies.
There has been a great interest in magnetic field induced quantum spin liquids in Kitaev magnets after the discovery of neutron scattering continuum and half quantized thermal Hall conductivity in the material $alpha$-RuCl$_3$. In this work, we provide a semiclassical analysis of the relevant theoretical models on large system sizes, and compare the results to previous studies on quantum models with small system sizes. We find a series of competing magnetic orders with fairly large unit cells at intermediate magnetic fields, which are most likely missed by previous approaches. We show that quantum fluctuations are typically strong in these large unit cell orders, while their magnetic excitations may resemble a scattering continuum and give rise to a large thermal Hall conductivity. Our work provides an important basis for a thorough investigation of emergent spin liquids and competing phases in Kitaev magnets.
We review recent progress in utilizing ultrafast light-matter interaction to control the macroscopic properties of quantum materials. Particular emphasis is placed on photoinduced phenomena that do not result from ultrafast heating effects but rather emerge from microscopic processes that are inherently nonthermal in nature. Many of these processes can be described as transient modifications to the free-energy landscape resulting from the redistribution of quasiparticle populations, the dynamical modification of coupling strengths and the resonant driving of the crystal lattice. Other pathways result from the coherent dressing of a materials quantum states by the light field. We discuss a selection of recently discovered effects leveraging these mechanisms, as well as the technological advances that led to their discovery. A road map for how the field can harness these nonthermal pathways to create new functionalities is presented.
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 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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