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Yongseong Choi

Publications and source records attributed to Yongseong Choi.

30 records · Page 2Linked to original sources

Evolution of structure and magnetism across the metal-insulator transition in the pyrochlore iridate $($Nd$_{1-x}$Ca$_x)_2$Ir$_2$O$_7$

We report on the evolution of the thermal metal-insulator transition in polycrystalline samples of Nd$_2$Ir$_2$O$_7$ upon hole-doping via substitution of Ca$^{2+}$ for Nd$^{3+}$. Ca substitution mediates a filling-controlled Mott-like transition with minimal resolvable structural changes and without altering site symmetry. Local structure confirms that Ca substitution does not result in local chemical phase separation, and absorption spectroscopy establishes that Ir cations maintain a spin-orbit entangled electronic configuration. The metal-insulator transition coincides with antiferromagnetic ordering on the Ir sublattice for all measured samples, and both decrease in onset temperature with Ca content. Weak low-temperature upturns in susceptibility and resistivity for samples with high Ca content suggest that Nd sublattice antiferromagnetism continues to couple to carriers in the metallic regime.

cond-mat.mtrl-sci↗

Photoemission and Dynamical Mean Field Theory Study of Electronic Correlation in a $t_{2g}^{5}$ Metal of SrRhO$_{3}$ Thin Film

Perovskite rhodates are characterized by intermediate strengths of both electronic correlation as well as spin-orbit coupling (SOC) and usually behave as moderately correlated metals. A recent publication (Phys. Rev. B 95, 245121(2017)) on epitaxial SrRhO$_3$ thin films unexpectedly reported a bad-metallic behavior and suggested the occurrence of antiferromagnetism below 100 K. We studied this SrRhO$_3$ thin film by hard x-ray photoemission spectroscopy and found a very small density of states (DOS) at Fermi level, which is consistent with the reported bad-metallic behavior. However, this negligible DOS persists up to room temperature, which contradicts with the explanation of antiferromagnetic transition at around 100 K. We also employed electronic structure calculations within the framework of density functional theory and dynamical mean-field theory. In contrast to the experimental results, our calculations indicate metallic behavior of both bulk SrRhO$_3$ and the SrRhO$_3$ thin film. The thin film exhibits stronger correlation effects than the bulk, but the correlation effects are not sufficient to drive a transition to an insulating state. The calculated uniform magnetic susceptibility is substantially larger in the thin film than that in the bulk. The role of SOC was also investigated and only a moderate modulation of the electronic structure was observed. Hence SOC is not expected to play an important role for electronic correlation in SrRhO$_3$.

cond-mat.str-el↗

Room-temperature ferromagnetic insulating state in highly cation-ordered epitaxial oxide double perovskite

Ferromagnetic insulators (FMIs) are one of the most important components in developing dissipationless electronic and spintronic devices. However, since ferromagnetism generally accompanies metallicity, FMIs are innately rare to find in nature. Here, novel room-temperature FMI films are epitaxially synthesized by deliberate control of the ratio of two B-site cations in the double perovskite Sr2FeReO6. In contrast to the known ferromagnetic metallic phase in stoichiometric Sr2FeReO6, a FMI state with a high Curie temperature (Tc~400 K) and a large saturation magnetization (MS~1.8 μB/f.u.) is found in highly cation-ordered Fe-rich phases. The stabilization of the FMI state is attributed to the formation of extra Fe3+-Fe3+ and Fe3+-Re6+ bonding states, which originate from the excess Fe. The emerging FMI state by controlling cations in the epitaxial oxide perovskites opens the door to developing novel oxide quantum materials & heterostructures.

cond-mat.mtrl-sci↗

Decoupling carrier concentration and electron-phonon coupling in oxide heterostructures observed with resonant inelastic x-ray scattering

We report the observation of multiple phonon satellite features in ultra thin superlattices of form $n$SrIrO$_3$/$m$SrTiO$_3$ using resonant inelastic x-ray scattering. As the values of $n$ and $m$ vary the energy loss spectra show a systematic evolution in the relative intensity of the phonon satellites. Using a closed-form solution for the cross section, we extract the variation in the electron-phonon coupling strength as a function of $n$ and $m$. Combined with the negligible carrier doping into the SrTiO$_3$ layers, these results indicate that tuning of the electron-phonon coupling can be effectively decoupled from doping. This work showcases both a feasible method to extract the electron-phonon coupling in superlattices and unveils a potential route for tuning this coupling which is often associated with superconductivity in SrTiO$_3$-based systems.

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↗

High pressure x-ray study of spin-Peierls physics in the quantum spin chain material TiOCl

The application of pressure can induce transitions between unconventional quantum phases in correlated materials. The inorganic compound TiOCl, composed of chains of S=1/2 Ti ions, is an ideal realization of a spin-Peierls system with a relatively simple unit cell. At ambient pressure, it is an insulator due to strong electronic interactions (a Mott insulator). Its resistivity shows a sudden decrease with increasing pressure, indicating a transition to a more metallic state which may coincide with the emergence of charge density wave order. Therefore, high pressure studies of the structure with x-rays are crucial in determining the ground-state physics in this quantum magnet. In ambient pressure, TiOCl exhibits a transition to an incommensurate nearly dimerized state at $T_{c2}=92$ K and to a commensurate dimerized state at $T_{c1}=66$ K. Here, we discover a rich phase diagram as a function of temperature and pressure using x-ray diffraction on a single crystal in a diamond anvil cell down to $T=4$ K and pressures up to 14.5 GPa. Remarkably, the magnetic interaction scale increases dramatically with increasing pressure, as indicated by the high onset temperature of the spin-Peierls phase. At $\sim$7 GPa, the extrapolated onset of the spin-Peierls phase occurs above $T=300$ K, indicating a quantum singlet state exists at room temperature. Further comparisons are made with the phase diagrams of related spin-Peierls systems that display metallicity and superconductivity under pressure.

cond-mat.str-el↗

Tuning Perpendicular Magnetic Anisotropy by Oxygen Octahedral Rotations in (La$_{1-x}$Sr$_{x}$MnO$_{3}$)/(SrIrO$_{3}$) Superlattices

Perpendicular magnetic anisotropy (PMA) plays a critical role in the development of spintronics, thereby demanding new strategies to control PMA. Here we demonstrate a conceptually new type of interface induced PMA that is controlled by oxygen octahedral rotation. In superlattices comprised of La$_{1-x}$Sr$_{x}$MnO$_{3}$ and SrIrO$_{3}$, we find that all superlattices (0$\leq$x$\leq$1) exhibit ferromagnetism despite the fact that La$_{1-x}$Sr$_{x}$MnO$_{3}$ is antiferromagnetic for x$>$0.5. PMA as high as 4$\times$10$^6$ erg/cm$^3$ is observed by increasing x and attributed to a decrease of oxygen octahedral rotation at interfaces. We also demonstrate that oxygen octahedral deformation cannot explain the trend in PMA. These results reveal a new degree of freedom to control PMA, enabling discovery of emergent magnetic textures and topological phenomena.

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↗

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↗

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↗

Competition between heavy-fermion and Kondo interaction in isoelectronic A-site ordered perovskites

With current research efforts shifting towards the 4$d$ and 5$d$ transition metal oxides, understanding the evolution of the electronic and magnetic structure as one moves away from 3$d$ materials is of critical importance. Here we perform X-ray spectroscopy and electronic structure calculations on $A$-site ordered perovskites with Cu in the $A$-site and the $B$-sites descending along the 9th group of the periodic table to elucidate the emerging properties as $d$-orbitals change from partially filled 3$d$, 4$d$, to 5$d$. The results show that when descending from Co to Ir the charge transfers from the cuprate like Zhang-Rice state on Cu to the t$_{2g}$ orbital of the B site. As the Cu $d$-orbital occupation approaches the Cu$^{2+}$ limit, a mixed-valence state in CaCu$_3$Rh$_4$O$_{12}$ and heavy fermion state in CaCu$_3$Ir$_4$O$_{12}$ are obtained. The investigated d-electron compounds are mapped onto the Doniach phase diagram of the competing RKKY and Kondo interactions developed for f-electron systems.

cond-mat.str-el↗

Critical phenomena of nano phase evolution in a first order transition

First order phase transitions occur discretely from one state to another, however they often display continuous behavior. To understand this nature, it is essential to probe how the emergent phase nucleates, interacts and evolves with the initial phase across the transition at microscopic scales. Here, the prototypical first-order magneto-structural transition in FeRh is used to investigate these phenomena. We find that the temperature evolution of the final phase exhibits critical behavior. Furthermore, a difference between the structure and magnetic transition temperatures reveals a novel intermediate phase created from the interface between the initial and nucleated final states. This emergent phase, characterized by its lack of spin order due to the competition between the antiferromagnetic and ferromagnetic interactions, leads to suppression of the dynamic aspect of the transition, generating a static mixed-phase-morphology. Understanding and controlling the transition process at this spatial scale is critical to optimizing functional device capabilities.

cond-mat.mes-hall↗