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S-W. Cheong

Publications and source records attributed to S-W. Cheong.

At least 19 recordsLinked to original sources

Orbital-specific Itinerancy and Localization in a Kagome Magnet

The kagome lattice naturally hosts flat bands, Dirac fermions, and van Hove singularities, yet whether its geometry can stabilize orbital-selective phases - a hallmark of Hund's physics in multi-orbital correlated systems - has remained an open question. Here, we combine resonant inelastic X-ray scattering with density functional theory and dynamical mean-field theory to demonstrate that YMn$_6$Sn$_6$ exhibits a spontaneous orbital differentiation into coexisting itinerant and localized electrons within the same Mn $3d$ manifold. Orbitals directed along Mn-Mn bonds provide coherent quasiparticles and metallic bands, while those pointing toward ligands become strongly correlated and display non-Fermi-liquid behavior. Hund's intra-atomic exchange suppresses orbital fluctuations, stabilizing this dichotomy and providing a natural double-exchange-like mechanism for the observed ferromagnetic bilayer coupling. Our work establishes YMn$_6$Sn$_6$ as a kagome platform where orbital selectivity, flat-band topology, and Hund's metallicity converge - revealing that geometric frustration and correlation-driven orbital differentiation can cooperatively design exotic quantum phases beyond the canonical paradigms of Mott physics or band topology alone.

cond-mat.str-el

Non-reciprocal circular dichroism of axial phonons coupled to ferro-rotational order

Circular dichroism (CD) in X-ray absorption, defined as the difference in absorption between opposite circular polarizations, is fundamentally enabled by the breaking of time-reversal symmetry or inversion symmetry. It is therefore sensitive to magnetism, chirality, and their interplay. In contrast, the sample symmetry alone is insufficient to determine whether CD in resonant inelastic X-ray scattering (RIXS) is allowed. Rather, RIXS-CD is governed by both the sample symmetry and the scattering geometry. Here, using RIXS, we identify circularly polarized phonons coupled to ferro-rotational order in MnTiO$_3$, which we refer to as ferro-axial phonons. Their excitations provide a direct demonstration of non-reciprocal RIXS-CD, in which the dichroic response changes upon reversing the propagation direction of the incident X-rays, although the system globally preserves both inversion and time-reversal symmetries. We propose that a condensate of these phonons, manifested as standing waves, underlies the ferro-rotational order in MnTiO$_3$. The observed non-reciprocal CD reflects the interplay among photon helicity, phonon polarization, and ferro-rotational order.

cond-mat.str-el

Bi-altermagnetism unveiled by sublattice-specific circular dichroism in resonant inelastic X-ray scattering

An altermagnet is a recently identified class of magnets that exhibit a zero net magnetic moment but break symmetry under the combined operations of parity and time reversal. It typically consists of two magnetic sites of opposite spins related by rotation within the unit cell. Here, we use circular dichroism (CD) in resonant inelastic X-ray scattering (RIXS) to identify a new form of altermagnetism, namely bi-altermagnetism, in the correlated insulator Fe2Mo3O8, which comprises two altermagnetic sublattices: one with alternating quasi-octahedral Fe environments and the other with alternating tetrahedral Fe environments. We experimentally revealed the emergence of CD in an achiral, zero-magnetization system, thereby probing mirror-symmetry breaking associated with altermagnetic order. Notably, the CD appeared at sublattice-specific excitations of the octahedral and tetrahedral sites, indicating symmetry breaking in both altermagnetic sublattices. Calculations based on a model with the bi-altermagnetic order along the c axis successfully reproduce the observed CD. Our findings provide compelling evidence for bi-altermagnetism in Fe2Mo3O8, and showcase the use of RIXS-CD as a probe of magnetic sublattices in systems with zero net magnetization.

cond-mat.str-el

Altermagnetic boosting of chiral phonons

Chirality characterizes the asymmetry between a structure and its mirror image and underlies a wide range of chiral functionalities. In crystallographically chiral materials, phonons with non-zero linear momentum $\textbf{k}$ can acquire a $k$-induced longitudinal magnetization, giving rise to chiral phonons. Helical spin order, with its proper screw-type configuration, breaks all mirror symmetries and therefore carries magnetic chirality. Such helical spins also generate non-relativistic spin splitting for any quasiparticle excitations propagating along the screw axis. To explore the possible connection between chiral phonons and magnetic chirality, we investigated the crystallographically polar and chiral compound (Mn,Ni)$_3$TeO$_6$, which hosts three distinct states: a paramagnetic state, a helical spin state with magnetic chirality, and a collinear spin state without magnetic chirality. We find an approximately tenfold enhancement of chiral-phonon coupling in the helical spin state along the screw axis, compared with both the paramagnetic and collinear spin states. These results identify a new route to amplify chiral phonons through an altermagnetic effect arising from the broken parity-time symmetry in helical spins. %from non-relativistic spin splitting.

cond-mat.str-el

Ferroaxial phonons in chiral and polar NiCo2TeO6

Perfect circular dichroism has been observed in the Raman scattering by the optical phonons in single chiral domain NiCo2TeO6 crystals. The selection rules for the optical phonons are determined by the combination of the chiral structure C and the electric polarization P along the c-axis. These two symmetry operations are equivalent to the ferroaxial order (C dot P) = A, so the observed optical phonons are referred to as "ferroaxial". For a given Raman scattering geometry the observed effect may also be described as a complete non-reciprocal propagation of the optical phonons, whose preferable vector direction is determined by the sign of C dot P. The combination of Raman scattering and polarization plane rotation of the transmitted white light allows for identification of the direction of electric polarization P in mono domain chiral crystals.

cond-mat.mtrl-sci

Effect of Coulomb interaction on the two-dimensional electronic structure of the van der Waals ferromagnet Cr$_2$Ge$_2$Te$_6$

In order to investigate the electronic properties of the semiconducting van der Waals ferromagnet Cr$_2$Ge$_2$Te$_6$ (CGT), where ferromagnetic layers are bonded through van der Waals forces, we have performed angle-resolved photoemission spectroscopy (ARPES) measurements and density-functional-theory (DFT+U) calculations. The valence-band maximum at the Γ point is located $\sim$ 0.2 eV below the Fermi level, consistent with the semiconducting property of CGT. Comparison of the experimental density of states with the DFT calculation has suggested that Coulomb interaction between the Cr 3d electrons U$_{\rm eff}$ $\sim$ 1.1 eV. The DFT+U calculation indicates that magnetic coupling between Cr atoms within the layer is ferromagnetic if Coulomb U $_{\rm eff}$ is smaller than 3.0 eV and that the inter-layer coupling is ferromagnetic below U$_{\rm eff}$ $\sim$ 1.0 eV. We therefore conclude that, for U$_{\rm eff}$ deduced by the experiment, the intra-layer Cr-Cr coupling is ferromagnetic and the inter-layer coupling is near the boundary between ferromagnetic and antiferromagnetic, which means experimentally deduced U$_{\rm eff}$ is consistent with theoretical ferromagnetic condition.

cond-mat.mtrl-sci

Toward the intrinsic limit of topological insulator Bi2Se3

Combining high resolution scanning tunneling microscopy and first principle calculations, we identified the major native defects, in particular the Se vacancies and Se interstitial defects that are responsible for the bulk conduction and nanoscale potential fluctuation in single crystals of archetypal topological insulator Bi2Se3. Here it is established that the defect concentrations in Bi2Se3 are far above the thermodynamic limit, and that the growth kinetics dominate the observed defect concentrations. Furthermore, through careful control of the synthesis, our tunneling spectroscopy suggests that our best samples are approaching the intrinsic limit with the Fermi level inside the band gap without introducing extrinsic dopants.

cond-mat.mtrl-sci

Terahertz Spin-Orbital Excitations in the paramagnetic state of multiferroic Sr$_2$FeSi$_2$O$_7$

We studied the novel multiferroic material Sr$_2$FeSi$_2$O$_7$, and found 3 absorption modes above the magnetic ordering transition temperature using time-domain terahertz spectroscopy. These absorption modes can be explained as the optical transitions between the spin-orbit coupling and crystal field split 3d$^6$ Fe$^{2+}$ ground state term in this material. Consideration of the compressed tetrahedral environment of the Fe$^{2+}$ site is crucial to understand the excitations. We point out, however, discrepancies between the single-site atomic picture and the experimental results.

cond-mat.str-el

Optical diode effect in the room-temperature multiferroic BiFeO$_3

Multiferroics permit the magnetic control of the electric polarization and electric control of the magnetization. These static magnetoelectric (ME) effects are of enormous interest: The ability to read and write a magnetic state current-free by an electric voltage would provide a huge technological advantage. Dynamic or optical ME effects are equally interesting because they give rise to unidirectional light propagation as recently observed in low-temperature multiferroics. This phenomenon, if realized at room temperature, would allow the development of optical diodes which transmit unpolarized light in one, but not in the opposite direction. Here, we report strong unidirectional transmission in the room-temperature multiferroic BiFeO$_3$ over the gigahertz--terahertz frequency range. Supporting theory attributes the observed unidirectional transmission to the spin-current driven dynamic ME effect. These findings are an important step toward the realization of optical diodes, supplemented by the ability to switch the transmission direction with a magnetic or electric field.

cond-mat.mtrl-sci

Hierarchical stripe phases in IrTe2 driven by competition between Ir dimerization and Te bonding

Layered 5d transition metal dichalcogenide (TMD) IrTe2 is distinguished from the traditional TMDs (such as NbSe2) by the existence of multiple CDW-like stripe phases and superconductivity at low temperatures. Despite of intensive studies, there is still no consensus on the physical origin of the stripe phases or even the ground state modulation for this 5d material. Here, we present atomic-scale evidence from scanning tunneling microscopy and spectroscopy (STM/STS), that the ground state of IrTe2 is a q=1/6 stripe phase, identical to that of the Se-doped compound. Furthermore, our data suggest that the multiple transitions and stripe phases are driven by the intralayer Ir-Ir dimerization that competes against the interlayer Te-Te bonding. The competition results in a unified phase diagram with a series of hierarchical modulated stripe phases, strikingly similar to the renowned "devil's staircase" phenomena.

cond-mat.str-el

Temperature-Dependent Interplay of Dzyaloshinskii-Moriya Interaction and Single-Ion Anisotropy in Multiferroic BiFeO$_3$

Low-energy magnon excitations in multiferroic BiFeO$_3$ were measured in detail as a function of temperature around several Brillouin zone centers by inelastic neutron scattering experiments on single crystals. Unique features around 1 meV are directly associated with the interplay of the Dzyaloshinskii-Moriya interaction and a small single-ion anisotropy. The temperature dependence of these and the exchange interactions were determined by fitting the measured magnon dispersion with spin-wave calculations. The spectra best fits an easy-axis type magnetic anisotropy and the deduced exchange and anisotropy parameters enable us to determine the anharmonicity of the magnetic cycloid. We then draw a direct connection between the changes in the parameters of spin Hamiltonian with temperature and the physical properties and structural deformations of BiFeO$_3$.

cond-mat.mtrl-sci

Spectral origin of the colossal magnetodielectric effect in multiferroic DyMn2O5

The origin of the colossal magnetodielectric effect in DyMn2O5 [1] has been an outstanding question in multiferroics. Here, we report the activation of the electric dipole mode at 4-5 cm-1 in an applied magnetic field which fully accounts for the CMD effect. We examine two alternative explanations of this mode: an electromagnon and transitions between f-electron levels of Dy3+ ions. The experimental and theoretical evidence supports the electromagnon origin of the CMD effect.

cond-mat.str-el

Weak ferromagnetic spin and charge stripe order in La[sub 5/3]Sr[sub 1/3]NiO[sub 4]

We present magnetization and specific heat data of a La5/3Sr1/3NiO4 single crystal in high magnetic fields. From the charge and spin stripe ordering temperatures, as well as a magnetic low temperature transition, we have constructed the electronic phase diagram for fields up to 14 Tesla. While the charge stripe ordering temperature TCO is independent of the magnetic field, there is a significant shift of the spin stripe ordering temperature TSO of about 1.5 K/ Tesla, if the magnetic fields are applied parallel to the NiO2-planes. The specific heat measurements indicate a large anomalous entropy change at TCO. In contrast, no significant entropy change is observed at the spin stripe transition. The high field magnetization experiments reveal the presence of in-plane weak ferromagnetic moments in the charge stripe ordered phase. From a phenomenological analysis, the magnetic correlation length of these moments is determined. We suggest that the weak ferromagnetism is due either to the presence of bond-centered charge stripes or to double exchange interactions across site-centered charge stripes.

cond-mat.str-el

Magnon breakdown in a two dimensional triangular lattice Heisenberg antiferromagnet of multiferroic LuMnO$_3$

The breakdown of magnons, the quasiparticles of magnetic systems, has rarely been seen. By using an inelastic neutron scattering technique we report the observation of spontaneous magnon decay in multiferroic LuMnO$_3$, a simple two-dimensional Heisenberg triangular lattice antiferromagnet, with large spin, S = 2. The origin of this rare phenomenon lies in the non-vanishing cubic interaction between magnons in the spin Hamiltonian arising from the noncollinear 120$^o$ spin structure. We observed all three key features of the nonlinear effects as theoretically predicted: a roton-like minimum, a flat mode, and a linewidth broadening, in our inelastic neutron scattering measurements of single crystal LuMnO$_3$. Our results show that quasiparticles in a system hitherto thought of as "classical" can indeed break down.

cond-mat.str-el

Hysteretic melting transition of a soliton lattice in a commensurate charge modulation

We report on the observation of the hysteretic transition of a commensurate charge modulation in IrTe$_2$ from transport and scanning tunneling microscopy (STM) studies. Below the transition ($T_{\rm C} \approx 275$ K on cooling) a $q = 1/5$ charge modulation was observed, which is consistent with previous studies. Additional modulations [$q_n = (3n+2)^{-1}$] appear below a second transition at $T_{\rm S}\approx 180$ K on cooling. The coexistence of various modulations persist up to $T_{\rm C}$ on warming. The atomic structures of charge modulations and the temperature dependent STM studies suggest that 1/5 modulation is a periodic soliton lattice which partially melts below $T_{\rm S}$ on cooling. Our results provide compelling evidence that the ground state of IrTe$_2$ is a commensurate 1/6 charge modulation, which originates from periodic dimerization of Te atoms visualized by atomically resolved STM images.

cond-mat.str-el

Negative magnetostrictive magnetoelectric coupling of BiFeO3

How the magnetoelectric coupling actually occurs on a microscopic level in multiferroic BiFeO3 is not well known. By using the high-resolution single crystal neutron diffraction techniques, we have determined the electric polarization of each individual elements of BiFeO3, and concluded that the magnetostrictive coupling suppresses the electric polarization at the Fe site below TN. This negative magnetoelectric coupling appears to outweigh the spin current contributions arising from the cycloid spin structure, which should produce a positive magnetoelectric coupling.

cond-mat.str-el

MnSb2O6: A polar magnet with a chiral crystal structure

Structural and magnetic chiralities are found to coexist in a small group of materials in which they produce intriguing phenomenologies such as the recently discovered skyrmion phases. Here, we describe a previously unknown manifestation of this interplay in MnSb2O6, a trigonal oxide with a chiral crystal structure. Unlike all other known cases, the MnSb2O6 magnetic structure is based on co-rotating cycloids rather than helices. The coupling to the structural chirality is provided by a magnetic axial vector, related to the so-called vector chirality. We show that this unique arrangement is the magnetic ground state of the symmetric-exchange Hamiltonian, based on ab-initio theoretical calculations of the Heisenberg exchange interactions, and is stabilised by out-of-plane anisotropy. MnSb2O6 is predicted to be multiferroic with a unique ferroelectric switching mechanism.

cond-mat.str-el

X-ray imaging and multiferroic coupling of cycloidal magnetic domains in ferroelectric monodomain BiFeO3

Magnetic domains at the surface of a ferroelectric monodomain BiFeO3 single crystal have been imaged by hard X-ray magnetic scattering. Magnetic domains up to several hundred microns in size have been observed, corresponding to cycloidal modulations of the magnetization along the wave-vector k=2π(δ,δ,0) and symmetry equivalent directions. The rotation direction of the magnetization in all magnetic domains, determined by diffraction of circularly polarized light, was found to be unique and in agreement with predictions of a combined approach based on a spin-model complemented by relativistic density-functional simulations. Imaging of the surface shows that the largest adjacent domains display a 120 degree vortex structure.

cond-mat.str-el