arXiv subjects

Young-June Kim

Publications and source records attributed to Young-June Kim.

At least 55 records · Page 3Linked to original sources

arXiv2018

Bulk-sensitive Imaging of Twin Domains in La$_{2-x}$Sr$_x$CuO$_4$ under Uniaxial Pressure

We report our study of twin domains in $La_{2-x}Sr_x CuO_4$ under uniaxial pressure. Using bulk-sensitive x-ray microdiffraction in Laue geometry, we image the distribution of twin domains at room temperature. When compressive uniaxial pressure is applied along one of the in-plane crystallographic axes, the domain population changes dramatically. We observe that the twin domain with shorter lattice parameter along the direction of pressure is unstable under compression, and disappears completely with only moderate pressure. On the other hand, application of tensile pressure changes the domain structure only slightly, demonstrating the asymmetric response of the sample to uniaxial pressure. Our observations suggest that a crystal's response to uniaxial pressure is complex and could deviate easily from the linear-response regime.

cond-mat.mtrl-sci↗

arXiv2018

Spin-orbit coupled systems in the "atomic" limit: rhenates, osmates, iridates

Motivated by RIXS experiments on a wide range of complex heavy oxides, including rhenates, osmates, and iridates, we discuss the theory of RIXS for site-localized $t_{2g}$ orbital systems with strong spin-orbit coupling. For such systems, we present exact diagonalization results for the spectrum at different electron fillings, showing that it accesses "single-particle" and "multi-particle" excitations. This leads to a simple picture for the energies and intensities of the RIXS spectra in Mott insulators such as double perovskites which feature highly localized electrons, and yields estimates of the spin-orbit coupling and Hund's coupling in correlated $5d$ oxides. We present new higher resolution RIXS data at the Re-L$_3$ edge in Ba$_2$YReO$_6$ which finds a previously unresolved peak splitting, providing further confirmation of our theoretical predictions. Using ab initio electronic structure calculations on Ba$_2$${\cal M}$ReO$_6$ (with ${\cal M}$=Re, Os, Ir) we show that while the atomic limit yields a reasonable effective Hamiltonian description of the experimental observations, effects such as $t_{2g}$-$e_g$ interactions and hybridization with oxygen are important. Our ab initio estimate for the strength of the intersite exchange coupling shows that, compared to the osmates, the exchange is one or two orders of magnitude weaker in the rhenates and iridates, which may partly explain the suppression of long-range magnetic order in the latter compounds. As a way to interpolate between the site-localized picture and our electronic structure band calculations, we discuss the spin-orbital levels of the ${\cal M}$O$_6$ cluster. This suggests a possible role for non-dispersive intra-cluster excitons in Ba$_2$YIrO$_6$ which may lead to a weak breakdown of the atomic $J_{\rm eff}=0$ picture and to small magnetic moments.

cond-mat.str-el↗

arXiv2018

From mean-field localized magnetism to itinerant spin fluctuations in the "Non-metallic metal" - FeCrAs

FeCrAs displays an unusual electrical response that is neither metallic in character nor divergent at low temperatures, as expected for an insulating response, and therefore it has been termed a "nonmetal-metal". We carried out neutron scattering experiments on powder and single crystal samples to study the magnetic dynamics and critical fluctuations in FeCrAs. Magnetic neutron diffraction measurements find Cr3+ magnetic order setting in at 115 K with the mean-field critical exponent. Neutron spectroscopy, however, observes gapless stiff magnetic fluctuations emanating from magnetic positions with propagation wave vector q_0=(1/3,1/3), which persists up to at least 80 meV. The magnetism in FeCrAs therefore displays a response which resembles that of itinerant magnets at high energy transfers, such as chromium alloys. We suggest that the presence of stiff high-energy spin fluctuations is the origin of the unusual temperature dependence of the resistivity.

cond-mat.str-el↗

arXiv2018

Probing electronic excitations in iridates with resonant inelastic x-ray scattering and emission spectroscopy techniques

We report a comprehensive resonant inelastic x-ray scattering (RIXS) study of various iridate materials focusing on core-level excitations and transitions between crystal-field split d-levels. The 2p core hole created at the Ir $L_3$ absorption edge has a very short lifetime giving rise to a broad absorption width ($\sim 5$~eV). This absorption linewidth broadening can be overcome by studying the resonant x-ray emission spectroscopy (RXES) map, which is a two-dimensional intensity map of the Ir L$α_2$ emission obtained with high energy-resolution monochromator and analyzer. By limiting the emitted photon energy to a narrow range, one can obtain x-ray absorption spectra in the high energy-resolution fluorescence detection (HERFD) mode, while one can also simulate quasi-$M_4$-edge absorption spectra by integrating over incident photon energies. Both methods improve the absorption line width significantly, allowing detailed studies of unoccupied electronic structure in iridates and other $5d$ transition metal compounds. On the other hand, the short lifetime of the 2p core hole benefits the study of excitations of valence electrons. We show that the incident energy dependence of the RIXS spectra for $d-d$ transitions is simple to understand due to the short core-hole lifetime, which validates ultra-short core-hole lifetime approximation used widely in theoretical calculations. We compared $d-d$ excitations in various iridates and found that the excitations between the t$_{2g}$ and e$_g$ states share many similarities among different materials. However, the RIXS spectra due to the transitions between the spin-orbit-split t$_{2g}$ levels vary widely depending on the oxidation state and electronic bandwidths.

cond-mat.str-el↗

arXiv2018

Pressure-driven collapse of the relativistic electronic ground state in a honeycomb iridate

The electronic ground state in many iridate materials is described by a complex wave-function in which spin and orbital angular momenta are entangled due to relativistic spin-orbit coupling (SOC). Such a localized electronic state carries an effective total angular momentum of $J_{eff}=1/2$. In materials with an edge-sharing octahedral crystal structure, such as the honeycomb iridates Li2IrO3 and Na2IrO3, these $J_{eff}=1/2$ moments are expected to be coupled through a special bond-dependent magnetic interaction, which is a necessary condition for the realization of a Kitaev quantum spin liquid. However, this relativistic electron picture is challenged by an alternate description, in which itinerant electrons are confined to a benzene-like hexagon, keeping the system insulating despite the delocalized nature of the electrons. In this quasi-molecular orbital (QMO) picture, the honeycomb iridates are an unlikely choice for a Kitaev spin liquid. Here we show that the honeycomb iridate Li2IrO3 is best described by a $J_{eff}=1/2$ state at ambient pressure, but crosses over into a QMO state under the application of small (~ 0.1 GPa) hydrostatic pressure. This result illustrates that the physics of iridates is extremely rich due to a delicate balance between electronic bandwidth, spin-orbit coupling, crystal field, and electron correlation.

cond-mat.str-el↗

arXiv2018

Evolution of Magnetic Excitations Across the Metal-Insulator Transition in a Pyrochlore Iridate Eu$_{2}$Ir$_{2}$O$_{7}$

We report Resonant Inelastic X-ray Scattering (RIXS) study of the magnetic excitation spectrum in a highly insulating Eu$_{2}$Ir$_{2}$O$_{7}$ single crystal that exhibits a metal-insulator transition at $T_{MI}$ = 111(7) K. A propagating magnon mode with 20 meV bandwidth and 28 meV magnon gap is found in the excitation spectrum at 7 K, which is expected in the all-in-all-out (AIAO) magnetically ordered state. This magnetic excitation exhibits substantial softening as temperature is raised towards $T_{MI}$, and turns into highly damped excitation in the paramagnetic phase. Remarkably, the softening occurs throughout the whole Brillouin zone including the zone boundary. This observation is inconsistent with magnon renormalization expected in a local moment system, and indicates that the strength of electron correlation in Eu$_{2}$Ir$_{2}$O$_{7}$ is only moderate, so that electron itinerancy should be taken into account in describing its magnetism.

cond-mat.str-el↗

arXiv2017

Determination of Hund's coupling in 5d Oxides using Resonant Inelastic X-ray Scattering

We report resonant inelastic X-ray scattering (RIXS) measurements on ordered double perovskite samples containing Re$^{5+}$ and Ir$^{5+}$ with $5d^2$ and $5d^4$ electronic configurations respectively. In particular, the observed RIXS spectra of Ba$_2$YReO$_6$ and Sr$_2$MIrO$_6$ (M=Y, Gd) show sharp intra-t$_{2g}$ transitions, which can be quantitatively understood using a minimal `atomic' Hamiltonian incorporating spin-orbit coupling ($λ$) and Hund's coupling ($J_H$). Our analysis yields $λ=0.38(2)$eV with $J_H=0.26(2)$eV for Re$^{5+}$, and $λ=0.42(2)$eV with $J_H=0.25(4)$eV for Ir$^{5+}$. Our results provide the first sharp estimates for the Hund's coupling in $5d$ oxides, and suggest that it should be treated on equal footing with spin-orbit interaction in multi-orbital $5d$ transition metal compounds.

cond-mat.str-el↗

arXiv2017

Phase Diagram of $α$-RuCl$_3$ in an in-plane Magnetic Field

The low-temperature magnetic phases in the layered honeycomb lattice material $α$-RuCl$_3$ have been studied as a function of in-plane magnetic field. In zero field this material orders magnetically below 7 K with so-called zigzag order within the honeycomb planes. Neutron diffraction data show that a relatively small applied field of 2 T is sufficient to suppress the population of the magnetic domain in which the zigzag chains run along the field direction. We found that the intensity of the magnetic peaks due to zigzag order is continuously suppressed with increasing field until their disappearance at $μ_o$H$_c$=8 T. At still higher fields (above 8 T) the zigzag order is destroyed, while bulk magnetization and heat capacity measurements suggest that the material enters a state with gapped magnetic excitations. We discuss the magnetic phase diagram obtained in our study in the context of a quantum phase transition.

cond-mat.str-el↗

arXiv2017

Large field-induced gap of Kitaev-Heisenberg paramagnons in $α$-RuCl$_{3}$

The honeycomb Kitaev-Heisenberg model is a source of a quantum spin liquid with Majorana fermions and gauge flux excitations as fractional quasiparticles. In the quest of finding a pertinent material, $α$-RuCl$_{3}$ recently emerged as a prime candidate. Here we unveil highly unusual low-temperature heat conductivity $κ$ of $α$-RuCl$_{3}$: beyond a magnetic field of $B_c\approx$ 7.5 T, $κ$ increases by about one order of magnitude, resulting in a large magnetic field dependent peak at about 7 K, both for in-plane as well as out-of-plane transport. This clarifies the unusual magnetic field dependence unambiguously to be the result of severe scattering of phonons off putative Kitaev-Heisenberg excitations in combination with a drastic field-induced change of the magnetic excitation spectrum. In particular, an unexpectedly large energy gap arises, which increases approximately linearly with the magnetic field and reaches a remarkably large $\hbarω_0/k_B\approx $ 50 K at 18 T.

cond-mat.str-el↗

arXiv2016

ARPES study of the Kitaev Candidate $α$-RuCl$_3$

$α$-RuCl$_3$ has been hinted as a spin-orbital-assisted Mott insulator in proximity to a Kitaev spin liquid state. Here we present ARPES measurements on single crystal $α$-RuCl$_3$ in both the pristine and electron-doped states, and combine them with LDA+SOC+U calculations performed for the several low-energy competing magnetically ordered states as well as the paramagnetic state. A large Mott gap is found in the measured band structure of the pristine compound that persists to more than 20 times beyond the magnetic ordering temperature, though the paramagnetic calculation shows almost no gap. Upon electron doping, spectral weight is transferred into the gap but the new states still maintain a sizable gap from the Fermi edge. These findings are most consistent with a Mott insulator with a somewhat exotic evolution out of the Mott state with both temperature and doping, likely related to unusually strong spin fluctuations.

cond-mat.str-el↗

arXiv2016

Disordered dimer state in electron-doped Sr$_{3}$Ir$_{2}$O$_{7}$

Spin excitations are explored in the electron-doped spin-orbit Mott insulator (Sr$_{1-x}$La$_{x}$)$_3$Ir$_2$O$_7$. As this bilayer square lattice system is doped into the metallic regime, long-range antiferromagnetism vanishes, yet a spectrum of gapped spin excitation remains. Excitation lifetimes are strongly damped with increasing carrier concentration, and the energy integrated spectral weight becomes nearly momentum independent as static spin order is suppressed. Local magnetic moments, absent in the parent system, grow in metallic samples and approach values consistent with one $J=\frac{1}{2}$ impurity per electron doped. Our combined data suggest that the magnetic spectra of metallic (Sr$_{1-x}$La$_{x}$)$_3$Ir$_2$O$_7$ are best described by excitations out of a disordered dimer state.

cond-mat.str-el↗

arXiv2016

Spin-orbit excitations and electronic structure of the putative Kitaev magnet $α$-RuCl$_3$

Mott insulators with strong spin-orbit coupling have been proposed to host unconventional magnetic states, including the Kitaev quantum spin liquid. The 4$d$ system $α$-RuCl$_3$ has recently come into view as a candidate Kitaev system, with evidence for unusual spin excitations in magnetic scattering experiments. We apply a combination of optical spectroscopy and Raman scattering to study the electronic structure of this material. Our measurements reveal a series of orbital excitations involving localized total angular momentum states of the Ru ion, implying that strong spin-orbit coupling and electron-electron interactions coexist in this material. Analysis of these features allows us to estimate the spin-orbit coupling strength, as well as other parameters describing the local electronic structure, revealing a well-defined hierarchy of energy scales within the Ru $d$ states. By comparing our experimental results with density functional theory calculations, we also clarify the overall features of the optical response. Our results demonstrate that $α$-RuCl$_3$ is an ideal material system to study spin-orbit coupled magnetism on the honeycomb lattice.

cond-mat.str-el↗

arXiv2015

Quasiparticle-continuum level repulsion in a quantum magnet

When the energy eigenvalues of two coupled quantum states approach each other in a certain parameter space, their energy levels repel each other and level crossing is avoided. Such level repulsion, or avoided level crossing, is commonly used to describe the dispersion relation of quasiparticles in solids. However, little is known about the level repulsion when more than two quasiparticles are present; for example, in an open quantum system where a quasiparticle can spontaneously decay into many particle continuum. Here we show that even in this case level repulsion exists between a long-lived quasiparticle state and a continuum. In our fine resolution neutron spectroscopy study of magnetic quasiparticles in a frustrated quantum magnet BiCu2PO6, we observe a renormalization of quasiparticle dispersion relation due to the presence of the continuum of multi-quasiparticle states. Our results have a broadimplication for understanding open quantum systems described by non-hermitian Hamiltonian.

cond-mat.str-el↗

arXiv2015

X-ray scattering study of pyrochlore iridates: crystal structure, electronic and magnetic excitations

We have investigated the structural, electronic, and magnetic properties of the pyrochlore iridates Eu2Ir2O7 and Pr2Ir2O7 using a combination of resonant elastic x-ray scattering, x-ray powder diffraction, and resonant inelastic x-ray scattering (RIXS). The structural parameters of Eu2Ir2O7 have been examined as a function of temperature and applied pressure, with a particular emphasis on regions of the phase diagram where electronic and magnetic phase transitions have been reported. We find no evidence of crystal symmetry change over the range of temperatures (~6 to 300 K) and pressures (~0.1 to 17 GPa) studied. We have also investigated the electronic and magnetic excitations in single crystal samples of Eu2Ir2O7 and Pr2Ir2O7 using high resolution Ir L3-edge RIXS. In spite of very different ground state properties, we find these materials exhibit qualitatively similar excitation spectra, with crystal field excitations at ~3-5 eV, spin-orbit excitations at ~0.5-1 eV, and broad low-lying excitations below ~0.15 eV. In Eu2Ir2O7 we observe highly damped magnetic excitations at ~45 meV, which display significant momentum dependence. We compare these results with recent dynamical structure factor calculations.

cond-mat.str-el↗

arXiv2015

Topological states in pyrochlore iridates: long-range anisotropy strongly competing with spin-orbit interaction

In the search for topological phases in correlated electron systems, iridium-based pyrochlores A2Ir2O7 -- materials with 5d transition-metal ions -- provide fertile grounds. Several novel topological states have been predicted but the actual realization of such states is believed to critically depend on the strength of local potentials arising from distortions of IrO6-cages. We test this hypothesis by measuring with resonant x-ray scattering the electronic level splittings in the A= Y, Eu systems, which we show to agree very well with ab initio electronic structure calculations. We find, however, that not distortions of IrO6-octahedra are the primary source for quenching the spin-orbit interaction, but strong long-range lattice anisotropies, which inevitably break the local cubic symmetry and will thereby be decisive in determining the system's topological ground state.

cond-mat.str-el↗

arXiv2015

Resonant inelastic x-ray scattering study of electronic excitations in insulating K$_{0.83}$Fe$_{1.53}$Se$_2$

We report an Fe $K$-edge resonant inelastic X-ray scattering (RIXS) study of K$_{0.83}$Fe$_{1.53}$Se$_2$. This material is an insulator, unlike many parent compounds of iron-based superconductors. We found a sharp excitation around 1 eV, which is resonantly enhanced when the incident photon energy is tuned near the pre-edge region of the absorption spectrum. The spectral weight and line shape of this excitation exhibit clear momentum dependence. In addition, we observe momentum-independent broad interband transitions at higher excitation energy of 3-7 eV. Calculations based on a 70 band $dp$ orbital model, using a moderate $U_{\rm eff}\approx 2.5$ eV, indicate that the $\sim$1 eV feature originates from the correlated Fe 3$d$ electrons, with a dominant $d_{xz}$ and $d_{yz}$ orbital character. We find that a moderate $U_{\rm eff}$ yields a satisfying agreement with the experimental spectra, suggesting that the electron correlations in the insulating and metallic iron based superconductors are comparable.

cond-mat.supr-con↗

arXiv2015

Magnetic order in $α$-RuCl$_3$: a honeycomb lattice quantum magnet with strong spin-orbit coupling

We report magnetic and thermodynamic properties of single crystal $α$-RuCl$_3$, in which the Ru$^{3+}$ ($4d^5$) ion is in its low spin state and forms a honeycomb lattice. Two features are observed in both magnetic susceptibility and specific heat data; a sharp peak at 7~K and a broad hump near 10-15K. In addition, we observe a metamagnetic transition between 5~T and 10~T. Our neutron diffraction study of single crystal samples confirms that the low temperature peak in the specific heat is associated with a magnetic order with unit cell doubling along the honeycomb (100) direction, which is consistent with zigzag order, one of the types of magnetic order predicted within the framework of the Kitaev-Heisenberg model.

cond-mat.str-el↗

arXiv2015

Scattering Continuum and Possible Fractionalized Excitations in $α$-RuCl$_3$

The combination of electronic correlation and spin-orbit coupling is thought to precipitate a variety of highly unusual electronic phases in solids, including topological and quantum spin liquid states. We report a Raman scattering study that provides evidence for unconventional excitations in $α$-RuCl$_3$, a spin-orbit coupled Mott insulator on the honeycomb lattice. In particular, our measurements reveal unusual magnetic scattering, typified by a broad continuum. The temperature dependence of this continuum is evident over a large scale compared to the magnetic ordering temperature, suggestive of frustrated magnetic interactions. This is confirmed through an analysis of the phonon linewidths, which show a related anomaly due to spin-phonon coupling. These observations are in line with theoretical expectations for the Heisenberg-Kitaev model and suggest that $α$-RuCl$_3$ may be close to a quantum spin liquid ground state.

cond-mat.str-el↗