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Huiwen Ji

Publications and source records attributed to Huiwen Ji.

At least 19 recordsLinked to original sources

Non-relativistic spin splitting in a triangular metal-excess magnet Fe$_{1+\delta}$Sb

Non-relativistic spin-splitting (NRSS) antiferromagnets have recently emerged as an important class of magnetic materials that combine compensated magnetism with momentum-dependent spin splitting, offering new opportunities for spintronic applications. Here, we investigate a NiAs-type Fe$_{1+\delta}$Sb series ($\delta = 0.17$-0.30) using neutron diffraction, pair distribution function, magnetometry and density functional theory calculations. Neutron diffraction establishes that Fe$_{1+\delta}$Sb adopts a $120^\circ$ coplanar compensated magnetic order with a non-zero propagation vector $\mathbf{k}=(1/3,\,1/3,\,0)$. Increasing interstitial Fe suppresses the ordered magnetic moment while inducing local symmetry lowering, as revealed by pair distribution function refinements. Density functional theory predicts momentum-dependent spin splitting, dominated by an out-of-plane spin polarization with an odd-parity f-wave-like symmetry, establishing the material as a non-collinear NRSS antiferromagnet. Motivated by the structural similarities between Fe$_{1+\delta}$Sb and a known altermagnet CrSb, we further investigate their solid solution and find that Cr substitution at intermediate concentrations gives rise to a ferromagnetic component and a cluster spin-glass behavior. These results establish Fe$_{1+\delta}$Sb as a new platform for non-collinear NRSS antiferromagnetism and demonstrate metal interstitial and substitution as effective parameters for tuning the magnetic order and properties.

cond-mat.mtrl-sci

Symmetry-Protected Weyl Nodal Loops in a Triangular Altermagnet

Weyl semimetals and altermagnets represent two distinct classes of quantum materials exhibiting nontrivial topological and magnetic order, respectively. Here we report the realization of a Weyl nodal-loop altermagnet in Cr$_7$Se$_8$, combining neutron diffraction and first-principles calculations. The hexagonal system hosts a coplanar $120^\circ$ compensated magnetic order on a triangular lattice, which breaks inversion-time-reversal and translation-time-reversal symmetries simultaneously while preserving a crystalline mirror plane. The resulting electronic structure features linearly dispersing nodal loops close to the Fermi level ($E_F$) confined to the mirror-invariant $k_z=0$ plane. Along high-symmetry directions, the crossings near $E_F$ form Dirac-like fourfold degeneracies in the absence of spin-orbit coupling; at generic momenta, these crossings split into twofold and form continuous Weyl-like nodal loops protected by mirror symmetry. The momentum-dependent spin polarization exhibits an $f$-wave-like pattern characteristic of odd-parity altermagnets.

cond-mat.mtrl-sci

La$_2$O$_3$Mn$_2$Se$_2$: a correlated insulating layered d-wave altermagnet

Altermagnets represent a new class of magnetic phases without net magnetization that are invariant under a combination of rotation and time reversal. Unlike conventional collinear antiferromagnets (AFM), altermagnets could lead to new correlated states and important material properties deriving from their non-relativistic spin-split band structure. Indeed, they are the magnetic analogue of unconventional superconductors and can yield spin polarized electrical currents in the absence of external magnetic fields, making them promising candidates for next-generation spintronics. Here, we report altermagnetism in the correlated insulator, magnetically-ordered tetragonal oxychalcogenide, La$_2$O$_3$Mn$_2$Se$_2$. Symmetry analysis reveals a $\mathit{d}_{x^2 - y^2}$-wave type spin momentum locking, which is supported by density functional theory (DFT) calculations. Magnetic measurements confirm the AFM transition below $\sim$166 K while neutron pair distribution function analysis reveals a 2D short-range magnetic order that persists above the Néel temperature. Single crystals are grown and characterized using X-ray diffraction, optical and electron microscopy, and microRaman spectroscopy to confirm the crystal structure, stoichiometry, and uniformity.

cond-mat.mtrl-sci

Noncentrosymmetric Triangular Magnet CaMnTeO$_6$: Strong Quantum Fluctuations and Role of s0 vs. s2 Electronic States in Competing Exchange Interactions

Noncentrosymmetric triangular magnets offer a unique platform for realizing strong quantum fluctuations. However, designing these quantum materials remains an open challenge attributable to a knowledge gap in the tunability of competing exchange interactions at the atomic level. Here, we create a new noncentrosymmetric triangular S = 3/2 magnet CaMnTeO$_6$ based on careful chemical and physical considerations. The model material displays competing magnetic interactions and features nonlinear optical responses with the capability of generating coherent photons. The incommensurate magnetic ground state of CaMnTeO$_6$ with an unusually large spin rotation angle of 127 deg.(1) indicates that the anisotropic interlayer exchange is strong and competing with the isotropic interlayer Heisenberg interaction. The moment of 1.39(1) $μ$B, extracted from low-temperature heat capacity and neutron diffraction measurements, is only 46% of the expected value of the static moment 3 $μ$B. This reduction indicates the presence of strong quantum fluctuations in the half-integer spin S = 3/2 CaMnTeO$_6$ magnet, which is rare. By comparing the spin-polarized band structure, chemical bonding, and physical properties of AMnTeO$_6$ (A = Ca, Sr, Pb), we demonstrate how quantum-chemical interpretation can illuminate insights into the fundamentals of magnetic exchange interactions, providing a powerful tool for modulating spin dynamics with atomically precise control.

cond-mat.str-el

Local electronic and magnetic properties of the doped topological insulators Bi$_{2}$Se$_{3}$:Ca and Bi$_{2}$Te$_{3}$:Mn investigated using ion-implanted $^{8}$Li $β$-NMR

We report $β$-detected nuclear magnetic resonance ($β$-NMR) measurements in Bi$_{2}$Se$_{3}$:Ca (BSC) and Bi$_{2}$Te$_{3}$:Mn (BTM) single crystals using $^{8}$Li$^{+}$ implanted to depths on the order of 100 nm. Above $\sim 200$ K, spin-lattice relaxation (SLR) reveals diffusion of $^{8}$Li$^{+}$, with activation energies of $\sim 0.4$ eV ($\sim 0.2$ eV) in BSC (BTM). At lower temperatures, the nuclear magnetic resonance (NMR) properties are those of a heavily doped semiconductor in the metallic limit, with Korringa relaxation and a small, negative, temperature-dependent Knight shift in BSC. From this, we make a detailed comparison with the isostructural tetradymite Bi$_{2}$Te$_{2}$Se (BTS) [McFadden et al., Phys Rev. B 99, 125201 (2019)]. In the magnetic BTM, the effects of the dilute Mn moments predominate, but remarkably the $^{8}$Li signal is not wiped out through the magnetic transition at 13 K, with a prominent critical peak in the SLR that is suppressed in a high applied field. This detailed characterization of the $^{8}$Li NMR response is an important step towards using depth-resolved $β$-NMR to study the low-energy properties of the chiral topological surface state (TSS). With the bulk NMR response now established in several Bi$_{2}$Ch$_{3}$ tetradymite topological insulators (TIs), the prospect of directly probing their chiral TSS using the depth resolution afforded by $β$-NMR remains strong.

cond-mat.mtrl-sci

The range of non-Kitaev terms and fractional particles in RuCl$_3$

Significant efforts have focused on the magnetic excitations of relativistic Mott insulators, predicted to realize the Kitaev quantum spin liquid (QSL). This exactly solvable model involves a highly entangled state resulting from bond-dependent Ising interactions that produce excitations which are non-local in terms of spin flips. A key challenge in real materials is identifying the relative size of the non-Kitaev terms and their role in the emergence or suppression of fractional excitations. Here, we identify the energy and temperature boundaries of non-Kitaev interactions by direct comparison of the Raman susceptibility of RuCl3 with quantum Monte Carlo (QMC) results for the Kitaev QSLs. Moreover, we further confirm the fractional nature of the magnetic excitations, which is given by creating a pair of fermionic quasiparticles. Interestingly, this fermionic response remains valid in the non-Kitaev range. Our results and focus on the use of the Raman susceptibility provide a stringent new test for future theoretical and experimental studies of QSLs.

cond-mat.str-el

Direct Evidence for Fermi Statistics from Proximity to the Kitaev Spin Liquid in RuCl3

A key characteristic of quantum spin liquids(QSL) is the presence of fractional excitations related to their entanglement properties, yet experimental verification of their statistics is missing. For example, in the potential Kitaev spin liquid, RuCl3 experiments uncovered signs of fractional particles, though not their Fermi statistics. Here we employ Raman scattering to reveal the true nature of the magnetic excitations, using improved experimental methods and analysis to remove the influence of laser heating and thermal fluctuations. Via the energy loss and gain spectra, we extract the energy and temperature dependence of the Raman susceptibility to prove RuCl3's magnetic response is given by pair creation of fermionic excitations. Furthermore, by comparing with quantum Monte Carlo (QMC) results for the exact Kitaev limit, we are able to discern the energy and temperature range where additional interaction terms are important. Our results open new directions in QSL research by providing a new way to investigate fractional excitations and the importance of terms causing spinon confinement.

cond-mat.str-el

Ionic and electronic properties of the topological insulator Bi$_2$Te$_2$Se investigated using $β$-detected nuclear magnetic relaxation and resonance of $^8$Li

We report measurements on the high temperature ionic and low temperature electronic properties of the 3D topological insulator Bi$_2$Te$_2$Se using ion-implanted $^8$Li $β$-detected nuclear magnetic relaxation and resonance. With implantation energies in the range 5-28 keV, the probes penetrate beyond the expected range of the topological surface state, but are still within 250 nm of the surface. At temperatures above ~150 K, spin-lattice relaxation measurements reveal isolated $^8$Li$^{+}$ diffusion with an activation energy $E_{A} = 0.185(8)$ eV and attempt frequency $τ_{0}^{-1} = 8(3) \times 10^{11}$ s$^{-1}$ for atomic site-to-site hopping. At lower temperature, we find a linear Korringa-like relaxation mechanism with a field dependent slope and intercept, which is accompanied by an anomalous field dependence to the resonance shift. We suggest that these may be related to a strong contribution from orbital currents or the magnetic freezeout of charge carriers in this heavily compensated semiconductor, but that conventional theories are unable to account for the extent of the field dependence. Conventional NMR of the stable host nuclei may help elucidate their origin.

cond-mat.mtrl-sci

Interacting multi-channel topological boundary modes in a quantum Hall valley system

Symmetry and topology play key roles in the identification of phases of matter and their properties. Both concepts are central to understanding quantum Hall ferromagnets (QHFMs), two-dimensional electronic phases with spontaneously broken spin or pseudospin symmetry whose wavefunctions also have topological properties. Domain walls between distinct broken symmetry QHFM phases are predicted to host gapless one-dimensional (1D) modes that emerge due to a topological change of the underlying electronic wavefunctions at such interfaces. Although a variety of QHFMs have been identified in different materials, probing interacting electronic modes at these domain walls has not yet been accomplished. Here we use a scanning tunneling microscope (STM) to directly visualize the spontaneous formation of boundary modes, within a sign-changing topological gap, at domain walls between different valley-polarized quantum Hall phases on the surface of bismuth. By changing the valley occupation and the corresponding number of modes at the domain wall, we can realize different regimes where the valley-polarized channels are either metallic or develop a spectroscopic gap. This behavior is a consequence of Coulomb interactions constrained by the symmetry-breaking valley flavor, which determines whether electrons in the topological modes can backscatter, making these channels a unique class of interacting Luttinger liquids.

cond-mat.mes-hall

Hidden structural order controls Li-ion transport in cation-disordered oxides for rechargeable lithium batteries

Crystal structures play a vital role in determining materials properties. In Li-ion cathodes, the crystal structure defines the dimensionality and connectivity of interstitial sites, thus determining Li-ion diffusion kinetics. While a perfect crystal has infinite structural coherence, a class of recently discovered high-capacity cathodes, Li-excess cation-disordered rocksalts, falls on the other end of the spectrum: Their cation sublattices are assumed to be randomly populated by Li and transition metal ions with zero configurational coherence based on conventional X-ray diffraction, such that the Li transport is purely determined by statistical effects. In contrast to this prevailing view, we reveal that cation short-range order, hidden in diffraction, is ubiquitous in these long-range disordered materials and controls the local and macroscopic environments for Li-ion transport. Our work not only discovers a crucial property that has previously been overlooked, but also provides new guidelines for designing and engineering disordered rocksalts cathode materials.

cond-mat.mtrl-sci

Ferroelectric quantum Hall phase revealed by visualizing Landau level wavefunction interference

Novel broken symmetry states can spontaneously form due to Coulomb interactions in electronic systems with multiple internal degrees of freedom. Multi-valley materials offer an especially rich setting for the emergence of such states, which have potential electronic and optical applications. To date, identification of these broken symmetry phases has mostly relied on the examination of macroscopic transport or optical properties. Here we demonstrate a powerful direct approach by visualizing the wave functions of bismuth surface states with a scanning tunneling microscope. Strong spin-orbit coupling on the surface of bismuth leads to six degenerate teardrop-shaped hole pockets. Our spectroscopic measurements reveal that this degeneracy is fully lifted at high magnetic field as a result of exchange interactions, and we are able to determine the nature of valley ordering by imaging the broken symmetry Landau level (LL) wave functions. The remarkable spatial features of singly degenerate LL wave functions near isolated defects contain unique signatures of interference between spin-textured valleys, which identify the electronic ground state as a quantum Hall ferroelectric. Our observations confirm the recent prediction that interactions in strongly anisotropic valley systems favor the occupation of a single valley, giving rise to emergent ferroelectricity in the surface state of bismuth.

cond-mat.mes-hall

Ir d-band Derived Superconductivity in the Lanthanum-Iridium System LaIr3

The electronic properties of the heavy metal superconductor LaIr3 are reported. The estimated superconducting parameters obtained from physical properties measurements indicate that LaIr3 is a BCS-type superconductor. Electronic band structure calculations show that Ir d- states dominate the Fermi level. A comparison of electronic band structures of LaIr3 and LaRh3 shows that the Ir-compound has a strong spin-orbit-coupling effect, which creates a complex Fermi surface.

cond-mat.supr-con

Discovery of intrinsic ferromagnetism in 2D van der Waals crystals

It has been long hoped that the realization of long-range ferromagnetic order in two-dimensional (2D) van der Waals (vdW) crystals, combined with their rich electronic and optical properties, would open up new possibilities for magnetic, magnetoelectric and magneto-optic applications. However, in 2D systems, the long-range magnetic order is strongly hampered by thermal fluctuations which may be counteracted by magnetic anisotropy, according to the Mermin-Wagner theorem. Prior efforts via defect and composition engineering, and proximity effect only locally or extrinsically introduce magnetic responses. Here we report the first experimental discovery of intrinsic long-range ferromagnetic order in pristine Cr2Ge2Te6 atomic layers by scanning magneto-optic Kerr microscopy. In such a 2D vdW soft ferromagnet, for the first time, an unprecedented control of transition temperature of ~ 35% - 57% enhancement is realized via surprisingly small fields (<= 0.3 Tesla in this work), in stark contrast to the stiffness of the transition temperature to magnetic fields in the three-dimensional regime. We found that the small applied field enables an effective anisotropy far surpassing the tiny magnetocrystalline anisotropy, opening up a sizable spin wave excitation gap. Confirmed by renormalized spin wave theory, we explain the phenomenon and conclude that the unusual field dependence of transition temperature constitutes a hallmark of 2D soft ferromagnetic vdW crystals. Our discovery of 2D soft ferromagnetic Cr2Ge2Te6 presents a close-to-ideal 2D Heisenberg ferromagnet for studying fundamental spin behaviors, and opens the door for exploring new applications such as ultra-compact spintronics.

cond-mat.mes-hall

High-Pressure Synthesis and Characterization of $β$-GeSe - A Semiconductor with Six-Rings in an Uncommon Boat Conformation

Two-dimensional materials have significant potential for the development of new devices. Here we report the electronic and structural properties of $β$-GeSe, a previously unreported polymorph of GeSe, with a unique crystal structure that displays strong two-dimensional structural features. $β$-GeSe is made at high pressure and temperature and is stable under ambient conditions. We compare it to its structural and electronic relatives $α$-GeSe and black phosphorus. The $β$ form of GeSe displays a boat conformation for its Ge-Se six-ring, while the previously known $α$ form, and black phosphorus, display the more common chair conformation for their six-rings. Electronic structure calculations indicate that $β$-GeSe is a semiconductor, with an approximate bulk band gap of $Δ~\approx$ 0.5 eV, and, in its monolayer form, $Δ~\approx$ 0.9 eV. These values fall between those of $α$-GeSe and black phosphorus, making $β$-GeSe a promising candidate for future applications. The resistivity of our $β$-GeSe crystals measured in-plane is on the order of $ρ\approx$ 1 $Ω$cm, while being essentially temperature independent.

cond-mat.mtrl-sci

Observation of a Nematic Quantum Hall Liquid on the Surface of Bismuth

Nematic quantum fluids with wavefunctions that break the underlying crystalline symmetry can form in interacting electronic systems. We examine the quantum Hall states that arise in high magnetic fields from anisotropic hole pockets on the Bi(111) surface. Spectroscopy performed with a scanning tunneling microscope shows that a combination of local strain and many-body Coulomb interactions lift the six-fold Landau level (LL) degeneracy to form three valley-polarized quantum Hall states. We image the resulting anisotropic LL wavefunctions and show that they have a different orientation for each broken-symmetry state. The wavefunctions correspond precisely to those expected from pairs of hole valleys and provide a direct spatial signature of a nematic electronic phase.

cond-mat.mes-hall

Magneto-Elastic Coupling in a potential ferromagnetic 2D Atomic Crystal

Cr2Ge2Te6 has been of interest for decades, as it is one of only a few naturally forming ferromagnetic semiconductors. Recently, this material has been revisited due to its potential as a 2 dimensional semiconducting ferromagnet and a substrate to induce anomalous quantum Hall states in topological insulators. However, many relevant properties of Cr2Ge2Te6 still remain poorly understood, especially the spin-phonon coupling crucial to spintronic, multiferrioc, thermal conductivity, magnetic proximity and the establishment of long range order on the nanoscale. We explore the interplay between the lattice and magnetism through high resolution micro-Raman scattering measurements over the temperature range from 10 K to 325 K. Strong spin-phonon coupling effects are confirmed from multiple aspects: two low energy modes splits in the ferromagnetic phase, magnetic quasielastic scattering in paramagnetic phase, the phonon energies of three modes show clear upturn below Tc, and the phonon linewidths change dramatically below Tc as well. Our results provide the first demonstration of spin-phonon coupling in a potential 2 dimensional atomic crystal.

cond-mat.mtrl-sci

A strong-topological-metal material with multiple Dirac cones

We report a new, cleavable, strong-topological-metal, Zr2Te2P, which has the same tetradymite-type crystal structure as the topological insulator Bi2Te2Se. Instead of being a semiconductor, however, Zr2Te2P is metallic with a pseudogap between 0.2 and 0.7 eV above the fermi energy (EF). Inside this pseudogap, two Dirac dispersions are predicted: one is a surface-originated Dirac cone protected by time-reversal symmetry (TRS), while the other is a bulk-originated and slightly gapped Dirac cone with a largely linear dispersion over a 2 eV energy range. A third surface TRS-protected Dirac cone is predicted, and observed using ARPES, making Zr2Te2P the first system to realize TRS-protected Dirac cones at M points. The high anisotropy of this Dirac cone is similar to the one in the hypothetical Dirac semimetal BiO2. We propose that if EF can be tuned into the pseudogap where the Dirac dispersions exist, it may be possible to observe ultrahigh carrier mobility and large magnetoresistance in this material.

cond-mat.mtrl-sci

Sn-doped Bi1.1Sb0.9Te2S, a bulk topological insulator with ideal properties

A long-standing issue in topological insulator research has been to find a material that provides an ideal platform for characterizing topological surface states without interference from bulk electronic states and can reliably be fabricated as bulk crystals. This material would be a bulk insulator, have a surface state Dirac point energy well isolated from the bulk valence and conduction bands, have high surface state electronic mobility, and be growable as large, high quality bulk single crystals. Here we show that this major materials obstacle in the field is overcome by crystals of lightly Sn-doped Bi1.1Sb0.9Te2S (Sn-BSTS) grown by the Vertical Bridgeman method, which we characterize here via angle-resolved photoemission spectroscopy, scanning tunneling microscopy, transport studies of the bulk and surface states, and X-ray diffraction and Raman scattering. We present this new material as a bulk topological insulator that can be reliably grown and studied in many laboratories around the world.

cond-mat.str-el