arXiv subjects

Young-June Kim

Publications and source records attributed to Young-June Kim.

At least 37 records · Page 2Linked to original sources

arXiv2023

Investigation of Cu-site disorder in undoped and doped BiCuSeO

We carried out X-ray diffraction and Extended X-ray Absorption Fine Structure (EXAFS) studies to investigate the origin of the low lattice thermal conductivity in BiCuSeO, and the role of silver (Ag) doping in doped samples. BiCuSeO is a promising thermoelectric material with high thermoelectric efficiency, which is significantly enhanced by doping either single Ag dopants or dual dopants (Pb and Ag). We verified that the thermal displacement parameters associated with copper (Cu) are significantly large in undoped BiCuSeO. Ag dopant, which replaces Cu, was also found to have similarly large thermal displacement parameters, that remain large down to low temperatures. Our results point towards significant disorder on Cu-site in both undoped and doped BiCuSeO, which is retained by Ag dopant on replacing Cu. The disorder is observed to be localized on the Cu-site and seems to be independent of other atoms in the crystal structure. Our observation of the disorder, which could be either static or quasi-static, is consistent with a rattling mode scenario.

cond-mat.mtrl-sci↗

arXiv2023

Oscillations in the magnetothermal conductivity of $\boldsymbolα$-RuCl$_3$: Evidence of transition anomalies

The 2D layered insulator $α$-RuCl$_3$ is a candidate material for a quantum spin-liquid state, which may be realized when a magnetic field suppresses the antiferromagnetic order present at low temperature. Oscillations in the field dependence of the thermal conductivity, observed for an in-plane magnetic field $B$ up to a critical field $B^{\star}$, have been attributed to exotic charge-neutral fermions, viewed as evidence of a quantum spin-liquid state between the critical field $B_{c}$ $\simeq 7$ T at which the antiferromagnetic phase ends and $B^{\star}$. Here we report measurements of the thermal conductivity of $α$-RuCl$_3$ as a function of magnetic field up to 15 T applied in two distinct in-plane directions: parallel and perpendicular to the Ru-Ru bond. We find that the number of oscillations between $B_{c}$ and $B^{\star}$ is the same for the two field directions even though the field interval between $B_{c}$ and $B^{\star}$ is different. In other words, the period of the oscillations is controlled by the transition fields $B_{c}$ and $B^{\star}$. We conclude that these are not true oscillations -- coming from putative fermions in a spin-liquid state -- but anomalies associated with a sequence of magnetic transitions.

cond-mat.str-el↗

arXiv2022

Acoustic phonon dispersion of $α$-RuCl$_3$

Acoustic phonons have recently been posited as playing an integral role in explaining the half-quantized thermal Hall effect in $α$-RuCl$_3$. Therefore, we present much needed inelastic x-ray scattering measurements of its acoustic phonon dispersion, along with calculations using the frozen-phonon method. We also discuss a temperature study which conclusively shows a first-order structural transition to a non-$C2/m$ space group at low temperature. Together these results are an important backbone for future theoretical and experimental studies of $α$-RuCl$_3$.

cond-mat.str-el↗

arXiv2022

Intermediate Valence State in $\mathrm{YbB_4}$ Revealed by Resonant X-ray Emission Spectroscopy

We report the temperature dependence of the Yb valence in the geometrically frustrated compound $\mathrm{YbB_4}$ from 12 to 300 K using resonant X-ray emission spectroscopy at the Yb $L_{α_1}$ transition. We find that the Yb valence, $v$, is hybridized between the $v=2$ and $v=3$ valence states, increasing from $v=2.61\pm0.01$ at 12 K to $v=2.67\pm0.01$ at 300 K, confirming that $\mathrm{YbB_4}$ is a Kondo system in the intermediate valence regime. This result indicates that the Kondo interaction in $\mathrm{YbB_4}$ is substantial, and is likely to be the reason why $\mathrm{YbB_4}$ does not order magnetically at low temperature, rather than this being an effect of geometric frustration. Furthermore, the zero-point valence of the system is extracted from our data and compared with other Kondo lattice systems. The zero-point valence seems to be weakly dependent on the Kondo temperature scale, but not on the valence change temperature scale $T_v$.

cond-mat.str-el↗

arXiv2022

Magnetic Excitations in Square Lattice Iridates: Contrast between Ba$_2$IrO$_4$ and Sr$_2$IrO$_4$

We report a resonant inelastic x-ray scattering (RIXS) investigation of ultra-thin epitaxial films of Ba$_2$IrO$_4$, and compare their low energy magnetic and spin-orbit excitations to those of their sister compound Sr$_2$IrO$_4$. Due to the 180$^\circ$ Ir-O-Ir bond, the bandwidth of the magnon and spin-orbiton is significantly larger in Ba$_2$IrO$_4$, making it difficult to describe these two types of excitations as separate well-defined quasiparticles. Both types of excitations are found to be quite sensitive to the effect of epitaxial strain. In addition, we find that the d-level inversion observed in Sr$_2$IrO$_4$ is absent in Ba$_2$IrO$_4$, as predicted in recent theoretical studies. Our results illustrate that the magnetic properties of Ba$_2$IrO$_4$ are substantially different from those of Sr$_2$IrO$_4$, suggesting that these materials need to be examined more carefully with electron itinerancy taken into account.

cond-mat.str-el↗

arXiv2022

Magnetic excitations in double perovskite iridates La$_{2}$$\mathit{M}$IrO$_{6}$ ($\mathit{M}$ = Co, Ni, and Zn) mediated by 3$\mathit{d}$-5$\mathit{d}$ hybridization

By performing resonant inelastic x-ray scattering (RIXS) measurements at the Ir $\mathit{L_{\mathrm{3}}}$ edge, we have investigated the low-energy elementary excitations in a series of double perovskite iridate single crystals, La$_{2}$$\mathit{M}$IrO$_{6}$ ($\mathit{M}$ = Co, Ni, and Zn). Almost dispersionless magnetic excitations at $\sim$ 42(6) meV and $\sim$ 35(5) meV have been observed in crystals containing magnetic 3$\mathit{d}$ ions, La$_{2}$CoIrO$_{6}$ and La$_{2}$NiIrO$_{6}$, respectively. In contrast, this low-energy magnetic excitation is absent in La$_{2}$ZnIrO$_{6}$ in which the 3$\mathit{d}$ ions are non-magnetic, suggesting the importance of 3$\mathit{d}$-5$\mathit{d}$ hybridization in the magnetic properties of these double perovskite iridates. The magnetic excitation is suppressed completely above the magnetic ordering temperature, suggesting the inadequacy of using a simple spin Hamiltonian to describe magnetism of these materials.

cond-mat.str-el↗

arXiv2021

Evidence of a Phonon Hall Effect in the Kitaev Spin Liquid Candidate $α$-RuCl$_3$

The material $α$-RuCl$_3$ has been the subject of intense scrutiny as a potential Kitaev quantum spin liquid, predicted to display Majorana fermions as low energy excitations. In practice, $α$-RuCl$_3$ undergoes a transition to a state with antiferromagnetic order below a temperature $T_{\rm N}$ $\approx$ 7 K, but this order can be suppressed by applying an external in-plane magnetic field of $H_\parallel$ = 7 T. Whether a quantum spin liquid phase exists just above that field is still an open question, but the reported observation of a quantized thermal Hall conductivity at $H_\parallel$ $>$ 7 T by Kasahara and co-workers $\big[$Kasahara ${\it et \ al}$., Nature ${\bf 559}$, 227 (2018)$\big]$ has been interpreted as evidence of itinerant Majorana fermions in the Kitaev quantum spin liquid state. In this study, we re-examine the origin of the thermal Hall conductivity $κ_{\rm xy}$ in $α$-RuCl$_3$. Our measurements of $κ_{\rm xy}$($T$) on several different crystals yield a temperature dependence very similar to that of the phonon-dominated longitudinal thermal conductivity $κ_{\rm xx}$($T$), for which the natural explanation is that $κ_{\rm xy}$ is also mostly carried by phonons. Upon cooling, $κ_{\rm xx}$ peaks at $T \simeq$ 20 K, then drops until $T_{\rm N}$, whereupon it suddenly increases again. The abrupt increase below $T_{\rm N}$ is attributed to a sudden reduction in the scattering of phonons by low-energy spin fluctuations as these become partially gapped when the system orders. The fact that $κ_{\rm xy}$ also increases suddenly below $T_{\rm N}$ is strong evidence that the thermal Hall effect in $α$-RuCl$_3$ is also carried predominantly by phonons. This implies that any quantized signal from Majorana edge modes would have to come on top of a sizable -- and sample-dependent -- phonon background.

cond-mat.str-el↗

arXiv2021

Neutron Scattering Study of Magnetic Anisotropy in a Tetragonal Antiferromagnet Bi$_2$CuO$_4$

We present a comprehensive study of magnon excitations in the tetragonal easy-plane anti-ferromagnet Bi$_2$CuO$_4$ using inelastic neutron scattering and spin wave analyses. The nature of low energy magnons, and hence the anisotropy in this material, has been controversial. We show unambiguously that the low energy magnon spectrum consists of a gapped and a gapless mode, which we attribute to out-of-plane and in-plane spin fluctuations, respectively. We modelled the observed magnon spectrum using linear spin wave analysis of a minimal anisotropic spin model motivated by the lattice symmetry. By studying the magnetic field dependence of the (1, 0, 0) Bragg peak intensity and the in-plane magnon intensity, we observed a spin-flop transition in the $ab$ plane at $\sim0.4$~T which directly indicates the existence of a small in-plane anisotropy that is classically forbidden. It is only by taking into account magnon zero-point fluctuations beyond the linear spin wave approximation, we could explain this in-plane anisotropy and its magnitude, the latter of which is deduced from critical field of the spin-flop transition. The microscopic origins of the observed anisotropic interactions are also discussed. We found that our data is inconsistent with a large Dzyaloshinskii-Moriya interaction, which suggests a potential departure of Bi$_2$CuO$_4$ from the conventional theories of magnetic anisotropy for other cuprates.

cond-mat.str-el↗

arXiv2021

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↗

arXiv2020

Bi$_{2}$Se$_{3}$ thin films heteroepitaxially grown on $α$-RuCl$_{3}$

Combining various two-dimensional materials into novel van der Waals (vdW) heterostructures has been shown to lead to new emergent quantum systems. A novel heterostructure composed of a vdW topological insulator (TI) such as Bi$_{2}$Se$_{3}$ with a quantum spin liquid (QSL) such as $α$-RuCl$_{3}$ is of great interest for the potential for the chiral Dirac electrons in the TI surface states to interact strongly with the fractionalized fermionic spin excitations in the QSL. We report the heteroepitaxial growth of Bi$_{2}$Se$_{3}$ thin films on $α$-RuCl$_{3}$ as well as the characterization of their structural and electrical properties. Bi$_{2}$Se$_{3}$ thin films with an atomically smooth and uniform surface are grown by molecular beam epitaxy. The heterostructure exhibits a preferential epitaxial relationship corresponding to $(5 \times 5)-$Bi$_{2}$Se$_{3}/(2\sqrt{3} \times 2\sqrt{3})R30°-α$-RuCl$_{3}$ commensurate supercells with a periodicity of 1.2 nm. The formation of the superlattice despite a lattice mismatch as large as 60% is attributed to the van der Waals heteroepitaxy. Magnetotransport measurements as a function of temperature show Bi$_{2}$Se$_{3}$ films grown on $α$-RuCl$_{3}$ are heavily $n$-doped, $n_{e}$ ~10$^{14}$ cm$^{-2}$, with mobility $μ$ ~450 cm$^{2}$ V$^{-1}$ s$^{-1}$ at low temperatures.

cond-mat.mtrl-sci↗

arXiv2020

Robust Long Range Magnetic Correlation across Anti-phase Domain Boundaries in Sr$_2$CrReO$_6$

Anti-site disorder is one of the most important issues that arises in synthesis of double perovskite for spintronic applications. Although it is known that anti-site disorder leads to a proliferation of structural defects, known as the anti-phase boundaries that separate ordered anti-phase domains in the sample, little is known about the magnetic correlation across these anti-phase boundaries on a microscopic level. Motivated by this, we report resonant elastic X-ray scattering study of room temperature magnetic and structural correlation in a thin-film sample of Sr$_2$CrReO$_6$, which has one of the highest $\mathrm{T_C}$ among double perovskites. Structurally, we discovered existence of anti-phase nanodomains of $\sim$15~nm in the sample. Magnetically, the ordered moments are shown to lie perpendicular to the $c$ direction. Most remarkably, we found that the magnetic correlation length far exceeds the size of individual anti-phase nanodomains. Our results therefore provide conclusive proof for existence of robust magnetic correlation across the anti-phase boundaries in Sr$_2$CrReO$_6$.

cond-mat.mes-hall↗

arXiv2020

Spin-Orbit Exciton in a Honeycomb Lattice Magnet CoTiO$_3$: Revealing Link Between Rare Earth and Transition Metal Magnetism

We carried out inelastic neutron scattering to study the spin-orbital (SO) exciton in a single crystal sample of CoTiO$_3$ as a function of temperature. CoTiO$_3$ is a honeycomb magnet with dominant XY-type magnetic interaction and an A-type antiferromagnetic order below $\mathrm{T_N} \approx 38$~K. We found that the SO exciton becomes softer, but acquires a larger bandwidth in the paramagnetic phase, compared to that in the magnetically ordered phase. Moreover, an additional mode is only observed in the intermediate temperature range, as the sample is warmed up above the lowest accessible temperature below $\mathrm{T_N}$. Such an unusual temperature dependence observed in this material suggests that its ground states (an $S_{\mathrm{eff}}=\frac{1}{2}$ doublet) and excited states multiplets are strongly coupled, and therefore cannot be treated independently, as often done in a pseudo-spin model. Our observations can be explained by a multi-level theory within random phase approximation that explicitly takes into account both the ground and excited multiplets. The success of our theory, which is originally developed to explain temperature dependence of magnetic excitations in the rare-earth magnets, highlight the similarity between the magnetic excitations in rare-earth systems and those in transition metal systems with strong spin orbit coupling.

cond-mat.str-el↗

arXiv2019

Ferromagnetic Kitaev interaction and the origin of large magnetic anisotropy in $α$-RuCl$_3$

$α$-RuCl$_3$ is drawing much attention as a promising candidate Kitaev quantum spin liquid. However, despite intensive research efforts, controversy remains about the form of the basic interactions governing the physics of this material. Even the sign of the Kitaev interaction (the bond-dependent anisotropic interaction responsible for Kitaev physics) is still under debate, with conflicting results from theoretical and experimental studies. The significance of the symmetric off-diagonal exchange interaction (referred to as the $Γ$ term) is another contentious question. Here, we present resonant elastic x-ray scattering data that provides unambiguous experimental constraints to the two leading terms in the magnetic interaction Hamiltonian. We show that the Kitaev interaction ($K$) is ferromagnetic, and that the $Γ$ term is antiferromagnetic and comparable in size to the Kitaev interaction. Our findings also provide a natural explanation for the large anisotropy of the magnetic susceptibility in $α$-RuCl$_3$ as arising from the large $Γ$ term. We therefore provide a crucial foundation for understanding the interactions underpinning the exotic magnetic behaviours observed in $α$-RuCl$_3$.

cond-mat.str-el↗

arXiv2019

Resonant inelastic x-ray scattering study of $α$-RuCl$_3$: a progress report

Ru M$_3$-edge resonant inelastic x-ray scattering (RIXS) measurements of RuCl$_3$ with 27 meV resolution reveals a spin-orbit exciton without noticeable splitting. We extract values for the spin-orbit coupling constant ($λ=154\pm2$ meV) and trigonal distortion field energy ($\left|Δ\right|<65$ meV) which support the $j_{\rm eff}=1/2$ nature of RuCl$_3$. We demonstrate the feasibility of M-edge RIXS for $4d$ systems, which allows ultra high-resolution RIXS of $4d$ systems until instrumentation for L-edge RIXS improves.

cond-mat.str-el↗

arXiv2019

Dirac magnons in a honeycomb lattice quantum XY magnet CoTiO3

The discovery of massless Dirac electrons in graphene and topological Dirac-Weyl materials has prompted a broad search for bosonic analogues of such Dirac particles. Recent experiments have found evidence for Dirac magnons above an Ising-like ferromagnetic ground state in a two-dimensional (2D) kagome lattice magnet and in the van der Waals layered honeycomb crystal CrI$_3$, and in a 3D Heisenberg magnet Cu$_3$TeO$_6$. Here we report on our inelastic neutron scattering investigation on large single crystals of a stacked honeycomb lattice magnet CoTiO$_3$, which is part of a broad family of ilmenite materials. The magnetically ordered ground state of CoTiO$_3$ features ferromagnetic layers of Co$^{2+}$, stacked antiferromagnetically along the $c$-axis. We discover that the magnon dispersion relation exhibits strong easy-plane exchange anisotropy and hosts a clear gapless Dirac cone along the edge of the 3D Brillouin zone. Our results establish CoTiO$_3$ as a model pseudospin-$1/2$ material to study interacting Dirac bosons in a 3D quantum XY magnet.

cond-mat.str-el↗

arXiv2019

Magnetic excitations in hole-doped Sr2IrO4: A comparison with electron-doped cuprates

We have studied the evolution of magnetic and orbital excitations as a function of hole-doping in single crystal samples of Sr2Ir(1-x)Rh(x)O4 (0.07 < x < 0.42) using high resolution Ir L3-edge resonant inelastic x-ray scattering (RIXS). Within the antiferromagnetically ordered region of the phase diagram (x < 0.17) we observe highly dispersive magnon and spin-orbit exciton modes. Interestingly, both the magnon gap energy and the magnon bandwidth appear to increase as a function of doping, resulting in a hardening of the magnon mode with increasing hole doping. As a result, the observed spin dynamics of hole-doped iridates more closely resemble those of the electron-doped, rather than hole-doped, cuprates. Within the paramagnetic region of the phase diagram (0.17 < x < 0.42) the low-lying magnon mode disappears, and we find no evidence of spin fluctuations in this regime. In addition, we observe that the orbital excitations become essentially dispersionless in the paramagnetic phase, indicating that magnetic order plays a crucial role in the propagation of the spin-orbit exciton.

cond-mat.str-el↗

arXiv2018

Neutron Scattering Investigation of Rhenium Orbital Ordering in $3d-5d$ Double Perovskite Ca$_2$FeReO$_6$

We have carried out inelastic neutron scattering experiments to study magnetic excitations in ordered double perovskite Ca$_2$FeReO$_6$. We found a well-defined magnon mode with a bandwidth of $\sim$50meV below the ferri-magnetic ordering temperature ($T_c\sim$520K), similar to previously studied Ba$_2$FeReO$_6$. The spin excitation is gapless for most temperatures within the magnetically ordered phase. However, a spin gap of $\sim$10meV opens up below $\sim$150K, which is well below the magnetic ordering temperature but coincides with a previously reported metal-insulator transition and onset of structural distortion. The observed temperature dependence of spin gap provides strong evidence for ordering of Re orbitals at $\sim$150~K, in accordance with earlier proposal put forward by Oikawa $\it{et.\,al}$ based on neutron diffraction [J. Phys. Soc. Jpn., $\bf{72}$, 1411 (2003)] as well as recent theoretical work by Lee and Marianetti [Phys. Rev. B, $\bf{97}$, 045102 (2018)]. The presence of separate orbital and magnetic ordering in Ca$_2$FeReO$_6$ suggests weak coupling between spin and orbital degrees of freedom and hints towards a sub-dominant role played by spin orbit coupling in describing its magnetism. In addition, we observed only one well-defined magnon band near magnetic zone boundary, which is incompatible with simple ferrimagnetic spin waves arising from Fe and Re local moments, but suggests a strong damping of Re magnon mode.

cond-mat.str-el↗

arXiv2018

Disorder induced power-law gaps in an insulator-metal Mott transition

A correlated material in the vicinity of an insulator-metal transition (IMT) exhibits rich phenomenology and variety of interesting phases. A common avenue to induce IMTs in Mott insulators is doping, which inevitably leads to disorder. While disorder is well known to create electronic inhomogeneity, recent theoretical studies have indicated that it may play an unexpected and much more profound role in controlling the properties of Mott systems. Theory predicts that disorder might play a role in driving a Mott insulator across an IMT, with the emergent metallic state hosting a power law suppression of the density of states (with exponent close to 1; V-shaped gap) centered at the Fermi energy. Such V-shaped gaps have been observed in Mott systems but their origins are as yet unknown. To investigate this, we use scanning tunneling microscopy and spectroscopy to study isovalent Ru substitutions in Sr$_3$(Ir$_{1-x}$Ru$_x$)$_2$O$_7$ which drives the system into an antiferromagnetic, metallic state. Our experiments reveal that many core features of the IMT such as power law density of states, pinning of the Fermi energy with increasing disorder, and persistence of antiferromagnetism can be understood as universal features of a disordered Mott system near an IMT and suggest that V-shaped gaps may be an inevitable consequence of disorder in doped Mott insulators.

cond-mat.str-el↗