arXiv subjects

H. -H. Kung

Publications and source records attributed to H. -H. Kung.

16 recordsLinked to original sources

arXiv2026

Electronic switching of topology in LaSbTe

In the past two decades, various classes of topological materials have been discovered, yet the deliberate control of topology in a single material remains largely unexplored. Here, we demonstrate full experimental control over the topological nodal loop in the square-net material LaSb$_x$Te$_{2-x}$ by chemical substitution and electron doping. Using angle-resolved photoemission spectroscopy (ARPES), we show that changing the antimony concentration x from 0.9 to 1.0 in the bulk opens a gap larger than 400~meV in the nodal loop. Symmetry analysis establishes that this effect originates from the breaking of \textit{n} glide symmetry in the square-net layer. Remarkably, the same topological phase transition can also be driven reversibly on the surface of LaSb$_x$Te$_{2-x}$ by \textit{in situ} chemical gating via potassium deposition, enabling on-demand switching of topology. The control parameter for both the bulk and surface transition is the electron concentration, providing a pathway towards applications based on switching topology by electrostatic gating.

cond-mat.mtrl-sci↗

arXiv2024

Spin-Mediated Direct Photon Scattering by Plasmons in BiTeI

We use polarization resolved Raman spectroscopy to demonstrate that for a 3D giant Rashba system the bulk plasmon collective mode can directly couple to the Raman response even in the long wavelength $\mathbf q \rightarrow 0$ limit. Although conventional theory predicts the plasmon spectral weight to be suppressed as the square of its quasi-momentum and thus negligibly weak in the Raman spectra, we observe a sharp in-gap plasmon mode in the Raman spectrum of BiTeI below the Rashba continuum. This coupling, in a polar system with spin-orbit coupling, occurs without assistance from phonons when the incoming photon excitation is resonant with Rashba-split intermediate states. We discuss the distinctive features of BiTeI's giant Rashba system band structure that enable the direct observation of plasmon in Raman scattering.

cond-mat.str-el↗

arXiv2024

Electronic and Vibrational Excitations on the Surface of the Three-Dimensional Topological Insulator Bi$_2$Te$_{3-x}$Se$_{x}$ (x = 0, 2, 3)

We study surface states in the three-dimensional topological insulators Bi$_2$Te$_{3-x}$Se$_{x}$ (x = 0, 2, 3) by polarization resolved resonant Raman spectroscopy. By tracking the spectral intensity of the surface phonon modes with respect to the incident photon energy, we show that the surface phonons are qualitatively similar to their bulk counterparts. Using the resonant Raman excitation profile, we estimated the binding energy of the surface conduction bands relative to bulk conduction bands. In addition, we selectively excite the surface-to-bulk electronic continuum near the Fermi energy in Bi$_2$Se$_3$ to determine the strength of Fano interaction between the most prominent surface phonon and the surface-to-bulk continuum.

cond-mat.mtrl-sci↗

arXiv2022

Optical manipulation of Rashba-split 2-Dimensional Electron Gas

In spintronic devices, the two main approaches to actively control the electrons' spin degree of freedom involve either static magnetic or electric fields. An alternative avenue relies on the application of optical fields to generate spin currents, which promises to bolster spin-device performance allowing for significantly faster and more efficient spin logic. To date, research has mainly focused on the optical injection of spin currents through the photogalvanic effect, and little is known about the direct optical control of the intrinsic spin splitting. Here, to explore the all-optical manipulation of a material's spin properties, we consider the Rashba effect at a semiconductor interface. The Rashba effect has long been a staple in the field of spintronics owing to its superior tunability, which allows the observation of fully spin-dependent phenomena, such as the spin-Hall effect, spin-charge conversion, and spin-torque in semiconductor devices. In this work, by means of time and angle-resolved photoemission spectroscopy (TR-ARPES), we demonstrate that an ultrafast optical excitation can be used to manipulate the Rashba-induced spin splitting of a two-dimensional electron gas (2DEG) engineered at the surface of the topological insulator Bi$_{2}$Se$_{3}$. We establish that light-induced photovoltage and charge carrier redistribution -- which in concert modulate the spin-orbit coupling strength on a sub-picosecond timescale -- can offer an unprecedented platform for achieving all optically-driven THz spin logic devices.

cond-mat.mes-hall↗

arXiv2022

Chiral Electronic Excitations in a Quasi-2D Rashba System BiTeI

The optical transitions between spin-polarized bands of the quasi-two dimensional Rashba system BiTeI are investigated using polarization resolved resonant Raman spectroscopy. We detect chiral excitations between states with opposite helicity and compare spectra to calculations within a three-band model. Using the resonant Raman excitation profile, we deduce the Rashba parameters and band gaps of the higher conduction bands near the Fermi level, and compare the parameters to values obtained by ab initio density function theory (DFT).

cond-mat.str-el↗

arXiv2021

Extremely large magnetoresistance from electron-hole compensation in the nodal loop semimetal ZrP$_2$

Several early transition metal dipnictides have been found to host topological semimetal states and exhibit large magnetoresistance. In this study, we use angle-resolved photoemission spectroscopy (ARPES) and magneto-transport to study the electronic properties of a new transition metal dipnictide ZrP$_2$. We find that ZrP$_2$ exhibits an extremely large and unsaturated magnetoresistance of up to 40,000 % at 2 K, which originates from an almost perfect electron-hole compensation. Our band structure calculations further show that ZrP$_2$ hosts a topological nodal loop in proximity to the Fermi level. Based on the ARPES measurements, we confirm the results of our calculations and determine the surface band structure. Our study establishes ZrP$_2$ as a new platform to investigate near-perfect electron-hole compensation and its interplay with topological band structures.

cond-mat.mtrl-sci↗

arXiv2019

Raman spectroscopy of $f$-electron metals: an example of CeB$_{6}$

We performed an optical spectroscopy study of electronic and magnetic excitations for a rare-earth system with a single electron quasi-localized in the f-shell on an ion at high-symmetry crystallographic site in application to CeB$_{6}$ heavy-fermion metal. We carried out group-theoretical classification of the electronic crystal field (CF) transitions and assessed their coupling to light cross-sections for polarization resolved Raman scattering processes. We discuss applicability of symmetrized Raman susceptibility to studies of exotic charge and spin high multiplet ordering phases in f-electron systems. We study temperature effects on intra- and inter-multiplet CF transitions and also on the coupling between the CF excitations with the lattice vibrations. We acquired temperature dependence of the low-frequency polarization resolved Raman response and obtained the static Raman susceptibility for all Raman-allowed symmetry channels: A$_{1g}$, E$_{g}$, T$_{1g}$, and T$_{2g}$ of the cubic O$_{h}$ point group. We demonstrate that for CeB$_{6}$ system only T$_{1g}$-symmetry static Raman susceptibility shows an anomalous temperature dependence which is consistent with the magnetic susceptibility data measured by other techniques. This anomalous behavior in the T$_{1g}$-channel signifies the presence of long wavelength magnetic fluctuations, while the lack of susceptibility enhancement for all the remaining symmetry channels indicates that long wavelength charge quadrupole fluctuations at low-temperature are weak.

cond-mat.str-el↗

arXiv2019

Observation of Chiral Surface Excitons in a Topological Insulator Bi$_2$Se$_3$

The protected electron states at the boundaries or on the surfaces of topological insulators (TIs) have been the subject of intense theoretical and experimental investigations. Such states are enforced by very strong spin-orbit interaction in solids composed of heavy elements. Here, we study the composite particles -- chiral excitons -- formed by the Coulomb attraction between electrons and holes residing on the surface of an archetypical three-dimensional topological insulator (TI), Bi$_2$Se$_3$. Photoluminescence (PL) emission arising due to recombination of excitons in conventional semiconductors is usually unpolarized because of scattering by phonons and other degrees of freedom during exciton thermalization. On the contrary, we observe almost perfectly polarization-preserving PL emission from chiral excitons. We demonstrate that the chiral excitons can be optically oriented with circularly polarized light in a broad range of excitation energies, even when the latter deviate from the (apparent) optical band gap by hundreds of meVs, and that the orientation remains preserved even at room temperature. Based on the dependences of the PL spectra on the energy and polarization of incident photons, we propose that chiral excitons are made from massive holes and massless (Dirac) electrons, both with chiral spin textures enforced by strong spin-orbit coupling. A theoretical model based on such proposal describes quantitatively the experimental observations. The optical orientation of composite particles, the chiral excitons, emerges as a general result of strong spin-orbit coupling in a 2D electron system. Our findings can potentially expand applications of TIs in photonics and optoelectronics.

cond-mat.mes-hall↗

arXiv2017

On the origin of critical nematic fluctuations in pnictide superconductors

We employ polarization-resolved Raman spectroscopy to study critical nematic fluctuations in Ba(Fe$_{1-x}$Au$_x$)$_2$As$_2$ superconductors above and across well separated tetragonal to orthorhombic phase transition at temperature $T_S(x)$ and the Néel transition at $T_N(x)$. The static Raman susceptibility in $XY$ symmetry channel increases upon cooling from room temperature following the Curie-Weiss law, with Weiss temperature $T_θ(x)$ several tens of degrees lower than $T_S(x)$. Data reveals a hidden nematic quantum critical point at $x_{c} = 0.031$ when the system becomes superconducting, indicating a direct connection between quantum critical nematic fluctuations and unconventional superconductivity. We attribute the origin of the nematicity to charge quadrupole fluctuations due to electron transfer between the nearly degenerate $d_{xz}/d_{yz}$ orbitals.

cond-mat.supr-con↗

arXiv2017

Anomalous magneto-elastic coupling in Au-doped BaFe2As2

We used polarization-resolved Raman scattering to study magneto-elastic coupling in Ba(Fe$_{1-x}$Au$_{x}$)$_2$As$_2$ crystals as a function of light Au-doping, materials for which temperatures of the structural transition ($T_S$) and of the magnetic ordering transition ($T_N$) split. We study the appearance of the $A_g$(As)phonon intensity in the $XY$ scattering geometry that is very weak just below $T_S$, but for which the intensity is significantly enhanced below $T_N$. In addition, the $A_g$(As) phonon shows an asymmetric line shape below $T_N$ and an anomalous linewidth broadening upon Au-doping in the magnetic phase. We demonstrate that the anomalous behavior of the $A_g$(As) phonon mode in the $XY$ scattering geometry can be consistently described by a Fano model involving the $A_g$(As) phonon mode interacting with the $B_{2g}$ symmetry-like magnetic continuum in which the magneto-elastic coupling constant is proportional to the magnetic order parameter.

cond-mat.supr-con↗

arXiv2017

Chiral Spin Mode on the Surface of a Topological Insulator

Using polarization-resolved resonant Raman spectroscopy, we explore collective spin excitations of the chiral surface states in a three dimensional topological insulator, Bi$_2$Se$_3$. We observe a sharp peak at 150 meV in the pseudovector $A_2$ symmetry channel of the Raman spectra. By comparing the data with calculations, we identify this peak as the transverse collective spin mode of surface Dirac fermions. This mode, unlike a Dirac plasmon or a surface plasmon in the charge sector of excitations, is analogous to a spin wave in a partially polarized Fermi liquid, with spin-orbit coupling playing the role of an effective magnetic field.

cond-mat.mtrl-sci↗

arXiv2017

Surface vibrational modes of the topological insulator Bi$_2$Se$_3$ observed by Raman spectroscopy

We present polarization resolved Raman scattering study of surface vibration modes in the topological insulator Bi$_2$Se$_3$ single crystal and thick films. Besides the four Raman active bulk phonons, we observed four additional modes with much weaker intensity and slightly lower energy than the bulk counterparts. Using symmetry analysis, we assigned these additional modes to out-of-plane surface phonons. Comparing with first principle calculations, we conclude that the appearance of these modes is due to $c$-axis lattice distortion and van der Waals gap expansion near the crystal surface. Two of the surface modes at 60 and 173 cm$^{-1}$ are associated with Raman active $A_{1g}$ bulk phonon modes, the other two at 136 and 158 cm$^{-1}$ are associated with infrared active bulk phonons with $A_{2u}$ symmetry. The latter become Raman allowed due to reduction of crystalline symmetry from $D_{3d}$ in the bulk to $C_{3v}$ on the crystal surface. In particular, the 158 cm$^{-1}$ surface phonon mode shows a Fano lineshape under resonant excitation, suggesting interference in the presence of electron-phonon coupling of the surface excitations.

cond-mat.mtrl-sci↗

arXiv2016

Analogy between the "Hidden Order" and the Orbital Antiferromagnetism in URu$_{2-x}$Fe$_x$Si$_2$

We study URu$_{2-x}$Fe$_x$Si$_2$, in which two types of staggered phases compete at low temperature as the iron concentration $x$ is varied: the nonmagnetic "hidden order" (HO) phase below the critical concentration $x_c$, and unconventional antiferromagnetic (AF) phase above $x_c$. By using polarization resolved Raman spectroscopy, we detect a collective mode of pseudovector-like $A_{2g}$ symmetry whose energy continuously evolves with increasing $x$; it monotonically decreases in the HO phase until it vanishes at $x=x_c$, and then reappears with increasing energy in the AF phase. The mode's evolution provides direct evidence for unified order parameter for both nonmagnetic and magnetic phases arising from the orbital degrees-of-freedom of the uranium-5$f$ electrons.

cond-mat.str-el↗

arXiv2016

Collective excitations of dynamic Fermi surface deformations in BaFe$_2$(As$_{0.5}$P$_{0.5}$)$_2$

We use electronic Raman scattering to study the low-energy excitations in BaFe$_2$(As$_{0.5}$P$_{0.5}$)$_2$ ($T_c \approx 16$ K) samples. In addition to a superconducting pair breaking peak (2$Δ=6.7$ meV) in the A$_{1g}$ channel with a linear tail towards zero energy, suggesting a nodal gap structure, we detect spectral features associated to Pomeranchuk oscillations in the A$_{1g}$, B$_{1g}$ and B$_{2g}$ channels. We argue that the small Fermi energy of the system is an essential condition for these Pomeranchuk oscillations to be underdamped. The Pomeranchuk oscillations have the same frequencies in the B$_{1g}$ and B$_{2g}$ channels, which we explain by the mixing of these symmetries resulting from the removal of the $σ_v$ and $σ_v$ symmetry planes due to a large As/P disorder. Interestingly, we show that the temperature at which the peaks corresponding to the Pomeranchuk oscillations get underdamped is consistent with the non-Fermi liquid to Femi liquid crossover determined by transport, suggesting that the Pomeranchuk instability plays an important role in the low-energy physics of the Fe-based superconductors.

cond-mat.supr-con↗

arXiv2016

Discovery of unconventional charge density wave at the surface of K0.9Mo6O17

We use Angle Resolved Photoemission Spectroscopy (ARPES), Raman spectroscopy, Low Energy Electron Diffraction (LEED) and x-ray scattering to reveal an unusual electronically mediated charge density wave (CDW) in K0.9Mo6O17. Not only does K0.9Mo6O17 lack signatures of electron-phonon coupling, but it also hosts an extraordinary surface CDW, with TS CDW =220 K nearly twice that of the bulk CDW, TB CDW =115 K. While the bulk CDW has a BCS-like gap of 12 meV, the surface gap is ten times larger and well in the strong coupling regime. Strong coupling behavior combined with the absence of signatures of strong electron-phonon coupling indicates that the CDW is likely mediated by electronic interactions enhanced by low dimensionality.

cond-mat.str-el↗

arXiv2014

Chirality density wave of the 'hidden order' phase in URu$_2$Si$_2$

A second-order phase transition is associated with emergence of an "order parameter" and a spontaneous symmetry breaking. For the heavy fermion superconductor URu$_2$Si$_2$, the symmetry of the order parameter associated with its ordered phase below 17.5 K has remained ambiguous despite 30 years of research, and hence is called "hidden order" (HO). Here we use polarization resolved Raman spectroscopy to specify the symmetry of the low energy excitations above and below the HO transition. These excitations involve transitions between interacting heavy uranium 5f orbitals, responsible for the broken symmetry in the HO phase. From the symmetry analysis of the collective mode, we determine that the HO parameter breaks local vertical and diagonal reflection symmetries at the uranium sites, resulting in crystal field states with distinct chiral properties, which order to a commensurate chirality density wave ground state.

cond-mat.str-el↗