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Jong-Woo Kim

Publications and source records attributed to Jong-Woo Kim.

At least 37 records · Page 2Linked to original sources

Local atomic configuration control of superconductivity in the undoped pnictide parent compound BaFe2As2

Emergent superconductivity is strongly correlated with the symmetry of local atomic configuration in the parent compounds of iron-based superconductors. While chemical doping or hydrostatic pressure can change the local geometry, these conventional approaches do not provide a clear pathway in tuning the detailed atomic arrangement predictably, due to the parent compounds complicated structural deformation in the presence of the tetragonal-to-orthorhombic phase transition. Here, we demonstrate a systematic approach to manipulate the local structural configurations in BaFe2As2 epitaxial thin films by controlling two independent structural factors orthorhombicity (in-plane anisotropy) and tetragonality (out-of-plane/in-plane balance) from lattice parameters. We tune superconductivity without chemical doping utilizing both structural factors separately, controlling local tetrahedral coordination in designed thin film heterostructures with substrate clamping and bi-axial strain. We further show that this allows quantitative control of both the structural phase transition, associated magnetism, and superconductivity in the parent material BaFe2As2. This approach will advance the development of tunable thin film superconductors in reduced dimension.

cond-mat.supr-con↗

A magnetic Weyl semimetallic phase in thin films of Eu$_2$Ir$_2$O$_7$

The interplay between electronic interactions and strong spin-orbit coupling is expected to create a plethora of fascinating correlated topological states of quantum matter. Of particular interest are magnetic Weyl semimetals originally proposed in the pyrochlore iridates, which are only expected to reveal their topological nature in thin film form. To date, however, direct experimental demonstrations of these exotic phases remain elusive, due to the lack of usable single crystals and the insufficient quality of available films. Here, we report on the discovery of the long-sought magnetic Weyl semi-metallic phase in (111)-oriented Eu$_2$Ir$_2$O$_7$ high-quality epitaxial thin films. The topological magnetic state shows an intrinsic anomalous Hall effect with colossal coercivity but vanishing net magnetization, which emerges below the onset of a peculiar magnetic phase with all-in-all-out antiferromagnetic ordering. The observed anomalous Hall conductivity arises from the non-zero Berry curvature emanated by Weyl node pairs near the Fermi level that act as sources and sinks of Berry flux, activated by broken cubic crystal symmetry at the top and bottom terminations of the thin film.

cond-mat.str-el↗

Strongly anisotropic antiferromagnetic coupling in EuFe2As2 revealed by stress detwinning

Of all parent compounds of iron-based high-temperature superconductors, EuFe2As2 exhibits by far the largest magnetostructural coupling due to the sizable biquadratic interaction between Eu and Fe moments. While the coupling between Eu antiferromagnetic order and Fe structural/antiferromagnetic domains enables rapid field detwinning, this prevents simple magnetometry measurements from extracting the critical fields of the Eu metamagnetic transition. Here we measure these critical fields by combining x-ray magnetic circular dichroism spectroscopy with in-situ tunable uniaxial stress and applied magnetic field. The combination of two tuning knobs allows us to separate the stress-detwinning of structural domains from the field-induced reorientation of Eu moments. Intriguingly, we find a spin-flip transition which can only result from a strongly anisotropic interaction between Eu planes. We argue that this anisotropic exchange is a consequence of the strong anisotropy in the magnetically ordered Fe layer, which presents a new form of higher-order coupling between Eu and Fe magnetism.

cond-mat.supr-con↗

Optical magnons with dominant bond-directional exchange interactions in a honeycomb lattice iridate $α$-Li$_{2}$IrO$_{3}$

We have used resonant inelastic x-ray scattering to reveal optical magnons in a honeycomb lattice iridate $α$-Li$_{2}$IrO$_{3}$. The spectrum in the energy region 20-25 meV exhibits momentum dependence, of which energy is highest at the location of the magnetic Bragg peak, ($\textit{h}, \textit{k}$) = ($\pm$0.32, 0), and lowered toward (0, 0) and ($\pm$1, 0). We compare our data with a linear spin-wave theory based on a generic nearest-neighbor spin model. We find that a dominant bond-directional Kitaev interaction of order 20 meV is required to explain the energy scale observed in our study. The observed excitations are understood as stemming from optical magnon modes whose intensity is modulated by a structure factor, resulting in the apparent momentum dependence. We also observed diffuse magnetic scattering arising from the short-range magnetic correlation well above $\textit{T}_{N}$. In contrast to Na$_{2}$IrO$_{3}$, this diffuse scattering lacks the $C_3$ rotational symmetry of the honeycomb lattice, suggesting that the bond anisotropy is far from negligible in $α$-Li$_{2}$IrO$_{3}$.

cond-mat.str-el↗

Self-Assembled Periodic Nanostructures Using Martensitic Phase Transformations

We describe a novel approach for the rational design and synthesis of self-assembled periodic nanostructures using martensitic phase transformations. We demonstrate this approach in a thin film of perovskite SrSnO3 with reconfigurable periodic nanostructures consisting of regularly spaced regions of sharply contrasted dielectric properties. The films can be designed to have different periodicities and relative phase fractions via chemical doping or strain engineering. The dielectric contrast within a single film can be tuned using temperature and laser wavelength, effectively creating a variable photonic crystal. Our results show the realistic possibility of designing large-area self-assembled periodic structures using martensitic phase transformations with the potential of implementing "built-to-order" nanostructures for tailored optoelectronic functionalities.

cond-mat.mtrl-sci↗

Strain-modulated Slater-Mott crossover of pseudospin-half square-lattice in (SrIrO3)1/ (SrTiO3)1 superlattices

We report on the epitaxial strain-driven electronic and antiferromagnetic modulations of a pseudospin-half square lattice realized in superlattices of (SrIrO3)1/(SrTiO3)1. With increasing compressive strain, we find the low-temperature insulating behavior to be strongly suppressed with a corresponding systematic reduction of both the Neel temperature and the staggered moment. However, despite such a suppression, the system remains weakly insulating above the Neel transition. The emergence of metallicity is observed under large compressive strain but only at temperatures far above the Néel transition. These behaviors are characteristics of the Slater-Mott crossover regime, providing a unique experimental model system of the spin-half Hubbard Hamiltonian with a tunable intermediate coupling strength.

cond-mat.str-el↗

Spontaneous Hall Effect enhanced by local Ir moments in epitaxial Pr$_2$Ir$_2$O$_7$ thin films

Rare earth pyrochlore Iridates (RE2Ir2O7) consist of two interpenetrating cation sublattices, the RE with highly-frustrated magnetic moments, and the Iridium with extended conduction orbitals significantly mixed by spin-orbit interactions. The coexistence and coupling of these two sublattices create a landscape for discovery and manipulation of quantum phenomena such as the topological Hall effect, massless conduction bands, and quantum criticality. Thin films allow extended control of the material system via symmetry-lowering effects such as strain. While bulk Pr2Ir2O7 shows a spontaneous hysteretic Hall effect below 1.5K, we observe the effect at elevated temperatures up to 15K in epitaxial thin films on (111) YSZ substrates synthesized via solid phase epitaxy. Similar to the bulk, the lack of observable long-range magnetic order in the thin films points to a topological origin. We use synchrotron-based element-specific x-ray diffraction (XRD) and x-ray magnetic circular dichroism (XMCD) to compare powders and thin films to attribute the spontaneous Hall effect in the films to localization of the Ir moments. We link the thin film Ir local moments to lattice distortions absent in the bulk-like powders. We conclude that the elevated-temperature spontaneous Hall effect is caused by the topological effect originating either from the Ir or Pr sublattice, with interaction strength enhanced by the Ir local moments. This spontaneous Hall effect with weak net moment highlights the effect of vanishingly small lattice distortions as a means to discover topological phenomena in metallic frustrated magnetic materials.

cond-mat.mtrl-sci↗

Epitaxial growth and antiferromagnetism of Sn-substituted perovskite iridate SrIr$_{0.8}$Sn$_{0.2}$O$_3$

5d iridates have shown vast emergent phenomena due to a strong interplay among its lattice, charge and spin degrees of freedom, because of which the potential in spintronic application of the thin-film form is highly leveraged. Here we have epitaxially stabilized perovskite SrIr$_{0.8}$Sn$_{0.2}$O$_3$ on [001] SrTiO$_3$ substrates through pulsed laser deposition and systematically characterized the structural, electronic and magnetic properties. Physical properties measurements unravel an insulating ground state with a weak ferromagnetism in the compressively strained epitaxial film. The octahedral rotation pattern is identified by synchrotron x-ray diffraction, resolving a mix of $a^+b^-c^-$ and $a^-b^+c^-$ domains. X-ray magnetic resonant scattering directly demonstrates a G-type antiferromagnetic structure of the magnetic order and the spin canting nature of the weak ferromagnetism.

cond-mat.mtrl-sci↗

Drastic suppression of superconducting $T_{c}$ by anisotropic strain near a nematic quantum critical point

High temperature superconductivity emerges in the vicinity of competing strongly correlated phases. In the iron-based superconductor $Ba(Fe_{1-x}Co_{x})_{2}As_{2}$, the superconducting state shares the composition-temperature phase diagram with an electronic nematic phase and an antiferromagnetic phase that break the crystalline rotational symmetry. Symmetry considerations suggest that anisotropic strain can enhance these competing phases and thus suppress the superconductivity. Here we study the effect of anisotropic strain on the superconducting transition in single crystals of $Ba(Fe_{1-x}Co_{x})_{2}As_{2}$ through electrical transport, magnetic susceptibility, and x-ray diffraction measurements. We find that in the underdoped and near-optimally doped regions of the phase diagram, the superconducting critical temperature is rapidly suppressed by both compressive and tensile stress, and in the underdoped case this suppression is enough to induce a strain-tuned superconductor to metal quantum phase transition.

cond-mat.supr-con↗

Anomalous Magnetoresistance due to Longitudinal Spin Fluctuations in a Jeff = 1/2 Mott Semiconductor

As a hallmark of electronic correlation, spin-charge interplay underlies many emergent phenomena in doped Mott insulators, such as high-temperature superconductivity, whereas the half-filled parent state is usually electronically frozen with an antiferromagnetic order that resists external control. We report on the observation of a new positive magnetoresistance that probes the staggered susceptibility of a pseudospin-half square-lattice Mott insulator built as an artificial SrIrO3/SrTiO3 superlattice. Its size is particularly large in the high-temperature insulating paramagnetic phase near the Néel transition. This novel magnetoresistance originates from a collective charge response to the large longitudinal spin fluctuations under a linear coupling between the external magnetic field and the staggered magnetization enabled by strong spin-orbit interaction. Our results demonstrate a magnetic control of the binding energy of the fluctuating particle-hole pairs in the Slater-Mott crossover regime analogous to the BCS-to-Bose-Einstein condensation crossover of ultracold-superfluids.

cond-mat.str-el↗

Giant magnetic response of a two-dimensional antiferromagnet

A fundamental difference between antiferromagnets and ferromagnets is the lack of linear coupling to a uniform magnetic field due to the staggered order parameter. Such coupling is possible via the Dzyaloshinskii-Moriya (DM) interaction but at the expense of reduced antiferromagnetic (AFM) susceptibility due to the canting-induced spin anisotropy. We solve this long-standing problem with a top-down approach that utilizes spin-orbit coupling in the presence of a hidden SU(2) symmetry. We demonstrate giant AFM responses to sub-Tesla external fields by exploiting the extremely strong two-dimensional critical fluctuations preserved under a symmetry-invariant exchange anisotropy, which is built into a square-lattice artificially synthesized as a superlattice of SrIrO3 and SrTiO3. The observed field-induced logarithmic increase of the ordering temperature enables highly efficient control of the AFM order. As antiferromagnets promise to afford switching speed and storage security far beyond ferromagnets, our symmetry-invariant approach unleashes the great potential of functional antiferromagnets.

cond-mat.str-el↗

Magnetism in artificial Ruddlesden-Popper iridates leveraged by structural distortions

We report on the tuning of magnetic interactions in superlattices composed of single and bilayer SrIrO$_3$ inter-spaced with SrTiO$_3$. Magnetic scattering shows predominately $c$-axis antiferromagnetic orientation of the magnetic moments for the bilayer justifying these systems as viable artificial analogues of the bulk Ruddlesden-Popper series iridates. Magnon gaps are observed in both superlattices, with the magnitude of the gap in the bilayer being reduced to nearly half that in its bulk structural analogue, Sr$_3$Ir$_2$O$_7$. We assign this to modifications in the anisotropic exchange driven by bending of the $c$-axis Ir-O-Ir bond and subsequent local environment changes, as detected by x-ray diffraction and modeled using spin wave theory. These findings explain how even subtle structural modulations driven by heterostructuring in iridates are leveraged by spin orbit coupling to drive large changes in the magnetic interactions.

cond-mat.str-el↗

Microscopic Observation of Entangled Multi-Magnetoelectric Coupling Phenomenon

Searching for new functionality in next generation electronic devices is a principal driver of material physics research. Multiferroics simultaneously exhibit electric and magnetic order parameters that may be coupled through magnetoelectric (ME) effects. In single-phase materials the ME effect arises from one of three known mechanisms: inverse Dzyaloshinskii-Moriya (IDM) interaction, spin dependent ligand-metal (p-d) orbital hybridization, and exchange striction. However, the coupling among these mechanisms remains largely unexplored despite envisioned potential capabilities. Here, we present cooperative tuning between both IDM interaction and p-d hybridization that leads to discrete ME states in Ba0.5Sr2.5Co2Fe24O41. In-situ x-ray diffraction exposes the microscopic interplay between these two mechanisms, marked by a unique ME susceptibility upon electric and magnetic fields. The entangled multi-ME coupling phenomenon observed in this room-temperature ME hexaferrite offers a pathway to novel functional control for ME device applications.

cond-mat.mtrl-sci↗

Effects of biaxial strain on the improper multiferroicity in h-LuFeO3 films

Elastic strain is potentially an important approach in tuning the properties of the improperly multiferroic hexagonal ferrites, the details of which have however been elusive due to the experimental difficulties. Employing the method of restrained thermal expansion, we have studied the effect of isothermal biaxial strain in the basal plane of h-LuFeO3 (001) films. The results indicate that a compressive biaxial strain significantly enhances the ferrodistortion, and the effect is larger at higher temperatures. The compressive biaxial strain and the enhanced ferrodistortion together, cause an increase in the electric polarization and a reduction in the canting of the weak ferromagnetic moments in h-LuFeO3, according to our first principle calculations. These findings are important for understanding the strain effect as well as the coupling between the lattice and the improper multiferroicity in h-LuFeO3. The experimental elucidation of the strain effect in h-LuFeO3 films also suggests that the restrained thermal expansion can be a viable method to unravel the strain effect in many other epitaxial thin film materials.

cond-mat.mtrl-sci↗

Atomic-scale control of magnetic anisotropy via novel spin-orbit coupling effect in La2/3Sr1/3MnO3/SrIrO3 superlattices

Magnetic anisotropy (MA) is one of the most important material properties for modern spintronic devices. Conventional manipulation of the intrinsic MA, i.e. magnetocrystalline anisotropy (MCA), typically depends upon crystal symmetry. Extrinsic control over the MA is usually achieved by introducing shape anisotropy or exchange bias from another magnetically ordered material. Here we demonstrate a pathway to manipulate MA of 3d transition metal oxides (TMOs) by digitally inserting non-magnetic 5d TMOs with pronounced spin-orbit coupling (SOC). High quality superlattices comprised of ferromagnetic La2/3Sr1/3MnO3 (LSMO) and paramagnetic SrIrO3 (SIO) are synthesized with the precise control of thickness at atomic scale. Magnetic easy axis reorientation is observed by controlling the dimensionality of SIO, mediated through the emergence of a novel spin-orbit state within the nominally paramagnetic SIO.

cond-mat.str-el↗

On the Structural Origin of the Single-ion Magnetic Anisotropy in LuFeO3

Electronic structures for the conduction bands of both hexagonal and orthorhombic LuFeO3 thin films have been measured using x-ray absorption spectroscopy at oxygen K (O K) edge. Dramatic differences in both the spectra shape and the linear dichroism are observed. These differences in the spectra can be explained using the differences in crystal field splitting of the metal (Fe and Lu) electronic states and the differences in O 2p-Fe 3d and O 2p-Lu 5d hybridizations. While the oxidation states has not changed, the spectra are sensitive to the changes in the local environments of the Fe3+ and Lu3+ sites in the hexagonal and orthorhombic structures. Using the crystal-field splitting and the hybridizations that are extracted from the measured electronic structures and the structural distortion information, we derived the occupancies of the spin minority states in Fe3+, which are non-zero and uneven. The single ion anisotropy on Fe3+ sites is found to originate from these uneven occupancies of the spin minority states via spin-orbit coupling in LuFeO3.

cond-mat.mtrl-sci↗

Novel electronic behavior driving NdNiO3 metal-insulator transition

We present evidence that the metal-insulator transition (MIT) in a tensile strained NdNiO3 (NNO) film is facilitated by a redistribution of electronic density and neither requires Ni charge disproportionation nor symmetry change [1, 2]. Given epitaxial tensile strain in thin NNO films induces preferential occupancy of the $e_g$ $d_{x^2-y^2}$ orbital ($s_{3z^2-r^2}$) we propose the larger transfer integral of this orbital state with the O 2p mediates a redistribution of electronic density from the Ni atom. A decrease in Ni $d_{x^2-y^2}$ orbital occupation is directly observed by resonant inelastic x-ray scattering below the MIT temperature. Furthermore, an increase in Nd charge occupancy is measured by x-ray absorption at the Nd L3 edge. Both spin-orbit coupling and crystal field effects combine to break the degeneracy of the Nd 5d states shifting the energy of the Nd $e_g$ $d_{x^2-y^2}$ orbital towards the Fermi level allowing the A site to become an active acceptor during the MI transition. This work identifies the relocation of electrons from the Ni 3d to the Nd 5d orbitals across the MIT. We propose the insulating gap opens between the Ni 3d and O 2p resulting from Ni 3d electron localization mediated by charge loss. The transition seems neither purely Mott-Hubbard nor simple charge transfer.

cond-mat.str-el↗

Direct Evidence for Dominant Bond-directional Interactions in a Honeycomb Lattice Iridate Na2IrO3

Heisenberg interactions are ubiquitous in magnetic materials and have been prevailing in modeling and designing quantum magnets. Bond-directional interactions offer a novel alternative to Heisenberg exchange and provide the building blocks of the Kitaev model, which has a quantum spin liquid (QSL) as its exact ground state. Honeycomb iridates, A2IrO3 (A=Na,Li), offer potential realizations of the Kitaev model, and their reported magnetic behaviors may be interpreted within the Kitaev framework. However, the extent of their relevance to the Kitaev model remains unclear, as evidence for bond-directional interactions remains indirect or conjectural. Here, we present direct evidence for dominant bond-directional interactions in antiferromagnetic Na2IrO3 and show that they lead to strong magnetic frustration. Diffuse magnetic x-ray scattering reveals broken spin-rotational symmetry even above Neel temperature, with the three spin components exhibiting nano-scale correlations along distinct crystallographic directions. This spin-space and real-space entanglement directly manifests the bond-directional interactions, provides the missing link to Kitaev physics in honeycomb iridates, and establishes a new design strategy toward frustrated magnetism.

cond-mat.mtrl-sci↗