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After the discovery of the ARECh2 (A=alkali or monovalent ions, RE=rare-earth, Ch= chalcogen) triangular lattice quantum spin liquid (QSL) family, a series of its oxide, sulfide, and selenide counterparts has been consistently reported and extensively investigated. While KErTe2 represents the initial synthesized telluride member, preserving its triangular spin lattice, it was anticipated that the substantial tellurium ions could impart more pronounced magnetic attributes and electronic structures to this material class. This study delves into the magnetism of KErTe2 at finite temperatures through magnetization and electron spin resonance (ESR) measurements. Based on the angular momentum $\hat{J}$ after spin-orbit coupling (SOC) and symmetry analysis, we obtain the magnetic effective Hamiltonian to describe the magnetism of Er3+ in R-3m space group. Applying the mean-field approximation to the Hamiltonian, we can simulate the magnetization and magnetic heat capacity of KErTe2 in paramagnetic state and determine the crystalline electric field (CEF) parameters and partial exchange interactions. The relatively narrow energy gaps between CEF ground state and excited states exert a significant influence on the magnetism. For example, small CEF excitations can result in a significant broadening of the ESR linewidth at 2 K. For the fitted exchange interactions, although the values are small, given a large angular momentum J = 15/2 after SOC, they still have a noticeable effect at finite temperatures. Notably, the heat capacity data under different magnetic fields along the c-axis direction also roughly match our calculated results, further validating the reliability of our analytical approach. These derived parameters serve as crucial tools for future investigations into the ground state magnetism of KErTe2., Comment: 11 pages, 6 figures

P-wave superconductors hold immense promise for both fundamental physics and practical applications due to their unusual pairing symmetry and potential topological superconductivity. However, the exploration of the p-wave superconductors has proved to be a complex endeavor. Not only are they rare in nature but also the identification of p-wave superconductors has been an arduous task in history. For example, phase-sensitive measurement, an experimental technique which can provide conclusive evidence for unconventional pairing, has not been implemented successfully to identify p-wave superconductors. Here, we study a recently discovered family of superconductors, A2Cr3As3 (A = K, Rb, Cs), which were proposed theoretically to be a candidate of p-wave superconductors. We fabricate superconducting quantum interference devices (SQUIDs) on exfoliated K2Cr3As3, and perform the phase-sensitive measurement. We observe that such SQUIDs exhibit a pronounced second-order harmonic component sin(2{\phi}) in the current-phase relation, suggesting the admixture of 0- and {\pi}-phase. By carefully examining the magnetic field dependence of the oscillation patterns of critical current and Shapiro steps under microwave irradiation, we reveal a crossover from 0- to {\pi}-dominating phase state and conclude that the existence of the {\pi}-phase is in favor of the p-wave pairing symmetry in K2Cr3As3.

Superconductivity involving finite momentum pairing can lead to spatial gap and pair density modulations, as well as Bogoliubov Fermi states within the superconducting gap. However, the experimental realization of their intertwined relations has been challenging. Here, we detect chiral kagome superconductivity modulations with residual Fermi arcs in KV3Sb5 and CsV3Sb5 by normal and Josephson scanning tunneling microscopy down to 30mK with resolved electronic energy difference at microelectronvolt level. We observe a U-shaped superconducting gap with flat residual in-gap states. This gap exhibits chiral 2 by 2 spatial modulations with magnetic field tunable chirality, which align with the chiral 2 by 2 pair density modulations observed through Josephson tunneling. These findings demonstrate a chiral pair density wave (PDW) that breaks time-reversal symmetry. Quasiparticle interference imaging of the in-gap zero-energy states reveals segmented arcs, with high-temperature data linking them to parts of the reconstructed V d-orbital states within the charge order. The detected residual Fermi arcs can be explained by the partial suppression of these d-orbital states through an interorbital 2 by 2 PDW and thus serve as candidate Bogoliubov Fermi states. Additionally, we differentiate the observed PDW order from impurity-induced gap modulations. Our observations not only uncover a chiral PDW order with orbital-selectivity, but also illuminate the fundamental space-momentum correspondence inherent in finite momentum paired superconductivity., Comment: To appear in Nature (2024)

Kagome superconductor CsV3Sb5, which exhibits intertwined unconventional charge density wave (CDW) and superconductivity, has garnered significant attention recently. Despite extensive static studies, the nature of these exotic electronic orders remains elusive. In this study, we investigate the non-equilibrium electronic structure of CsV3Sb5 via time- and angle-resolved photoemission spectroscopy. Our results reveal that upon laser excitation, the van Hove singularities immediately shift towards the Fermi level and subsequently oscillate in sync with a 1.3 THz coherent phonon mode. By analyzing the coherent intensity oscillations in the energy-momentum (E-k) map, we find that this coherent phonon is strongly coupled with electronic bands from both Sb and V orbitals. While typically observable only in the CDW state, remarkably, we find that the 1.3-THz coherent phonon mode can be persistently excited at temperatures above T_CDW, suggesting the potential existence of fluctuated CDW in CsV3Sb5. These findings enhance our understanding of the unconventional CDW control of kagome superconductivity., Comment: 11 pages, 5 figures

The process how heavy-electron state is established in Kondo-lattice compounds remains an unsolved issue. Recent angle-resolved photoemission spectroscopy and ultrafast optical spectroscopy imply an intermediate regime with hybridization fluctuations prior to the establishment of Kondo coherence, which appears at odds with traditional transport measurements. Extensive experimental works are highly demanded to both reconcile this dichotomy and delineate the intrinsic features in this special regime. Here, on the example of quasi-one-dimensional Kondo lattice compound CeCo$_2$Ga$_8$, we investigated angular dependent magnetotransport properties by planar Hall effect and planar anisotropic magnetoresistance measurements. Upon cooling from $T_K^{on}$ (an onset of incoherent Kondo scattering ) to below $T^*$ (where coherent $c$-$f$ hybridization comes into play), the two-fold symmetrical pattern of planar Hall effect changes sign gradually (i.e. $180^\circ$ phase shift); most strikingly, as a crossover, additional oscillations appear and persist until the heavy-electron state is stabilized below $T^*$. These results provide new insights for the regime of hybridization dynamics which might be deemed as a precursor state of the heavy-electron state., Comment: 19 pages, 4 figures

In recent decades, there has been a persistent pursuit of applications for surface/edge states in topological systems, driven by their dissipationless transport effects. However, there have been limited tangible breakthroughs in this field. This work demonstrates the remarkable properties of the topological insulator Ta2Pd3Te5, as a thermometer. This material exhibits a power-law correlation in temperature-dependent resistance at low temperatures, stemming from its Luttinger liquid behavior of edge states, while exhibiting semiconductor behavior at high temperatures. The power-law behavior effectively addresses the issue of infinite resistance in semiconductor thermometers at ultra-low temperatures, thereby playing a crucial role in enabling efficient thermometry in refrigerators supporting millikelvin temperatures or below. By employing chemical doping, adjusting thickness, and controlling gate voltage, its power-law behavior and semiconductor behavior can be effectively modulated. This enables efficient thermometry spanning from millikelvin temperatures to room temperature, and allows for precise local temperature measurement. Furthermore, this thermometer exhibits excellent temperature sensitivity and resolution, and can be fine-tuned to show small magnetoresistance. In summary, the Ta2Pd3Te5 thermometer, also referred to as a topological thermometer, exhibits outstanding performance and significant potential for measuring a wider range of temperatures compared to conventional low-temperature thermometers., Comment: 15 pages, 9 figures

Multiferroic materials, which simultaneously exhibit ferroelectricity and magnetism, have attracted substantial attention due to their fascinating physical properties and potential technological applications. With the trends towards device miniaturization, there is an increasing demand for the persistence of multiferroicity in single-layer materials at elevated temperatures. Here, we report high-temperature multiferroicity in single-layer CuCrSe$_2$, which hosts room-temperature ferroelectricity and 120 K ferromagnetism. Notably, the ferromagnetic coupling in single-layer CuCrSe$_2$ is enhanced by the ferroelectricity-induced orbital shift of Cr atoms, which is distinct from both types I and II multiferroicity. These findings are supported by a combination of second-harmonic generation, piezo-response force microscopy, scanning transmission electron microscopy, magnetic, and Hall measurements. Our research provides not only an exemplary platform for delving into intrinsic magnetoelectric interactions at the single-layer limit but also sheds light on potential development of electronic and spintronic devices utilizing two-dimensional multiferroics.

We report the magnetic properties of newly synthesized, single crystals of $\mathrm{TbTi_3Bi_4}$ whose crystal structure is highlighted by the stacking of terbium-based zigzag chains and titanium-based kagome lattices. This compound demonstrates extreme easy-axis magnetic anisotropy due to the crystalline-electric-field effect which aligns the $\mathrm{Tb^{3+}}$ moments along the zigzag chain direction. As the result of the strong single-ion anisotropy and multiple magnetic interactions, $\mathrm{TbTi_3Bi_4}$ behaves as a quasi-one-dimensional Ising magnet with a remarkable antiferromagnetic ordering at $T_\mathrm{N}$ = 20.4 K. When a magnetic field is applied along the direction of the zigzag chain, multiple meta-magnetic transitions occur between 1/3 and other magnetization plateaus. We have created a field-temperature phase diagram and mapped out the complex magnetic structures resulting from frustration., Comment: 10 pages, 10 figures

The emerging all-van der Waals (vdW) magnetic heterostructure provides a new platform to control the magnetization by the electric field beyond the traditional spintronics devices. One promising strategy is using unconventional spin-orbit torque (SOT) exerted by the out-of-plane polarized spin current to enable deterministic magnetization switching and enhance the switching efficiency. However, in all-vdW heterostructures, large unconventional SOT remains elusive and the robustness of the field-free switching against external magnetic field hasn't been examined, which hinder further applications. Here we demonstrate the field-free switching in an all-vdW heterostructure combining a type-II Weyl semimetal TaIrTe4 and above-room-temperature ferromagnet Fe3GaTe2. The fully field-free switching can be achieved at 2.56 x 10^10 A per m2 at 300K and a large SOT effective field efficiency of the out-of-plane polarized spin current generated by TaIrTe4 is determined to be 0.37. Moreover, we find that the switching polarity cannot be changed until the external in-plane magnetic field reaches 252mT, indicating a robust switching against the magnetic field. The numerical simulation suggests the large unconventional SOT reduces the switching current density and enhances the robustness of the switching. Our work shows that all-vdW heterostructures are promising candidates for future highly efficient and stable SOT-based devices., Comment: 15 pages, 4 figures, accepted by Advanced Materials

Combining high-throughput first-principles calculations and experimental measurements, we have identified a novel family of fast lithium-ion chalcogenide conductors in Li$_2$BMQ$_4$ (2114, B = Ca, Sr and Ba; M = Si, Ge and Sn; Q = O, S and Se) systems. Our calculations demonstrate that most of the thermodynamically and kinetically stable sulfides and selenides in this new system exhibit ultralow Li$^+$ ion migration activation energy (0.16 eV ~ 0.56 eV) and considerable bandgaps varying between ~ 2 eV and 3.5 eV. We have successfully synthesized Li$_2$BaSnS$_4$ and Li$_2$SrSiS$_4$, and they exhibit excellent moisture stability through H$_2$S gas measurements. Electrochemical impedance measurements indicate 2114 systems show the typical features of solid ionic conductors, with a room-temperature Li$^+$ conductivity close to 5$\times$10$^{-4}$ mS/cm aligning with our molecular dynamics simulations. Furthermore, we have theoretically investigated the substitution of Cl$^-$ at S$^{2-}$ site. The doped compounds display significantly higher conductivity, with an increase of about three orders of magnitude (up to a maximum of 0.72 mS/cm) compared to the undoped compounds. These findings offer valuable insights for the further exploration of potential chalcogenide solid electrolyte materials with robust air stability and enhanced ionic conductivity for practical applications in lithium-ion batteries.

Utilizing ultrafast time-resolved pump-probe spectroscopy measurements, we investigate the photoinduced quasiparticle dynamics of the topological materials LaSbTe and CeSbTe. In LaSbTe, the relaxation of quasiparticles is dominated by two different mechanisms: electron-phonon coupling, and phonon-assisted electron-hole recombination. Significantly, the amplitude of photoinduced reflectivity related to the former one shows two pronounced peaks at 156 K and 263 K, indicating the occurrence of two charge density wave (CDW) phase transitions. The ultrafast responses of CeSbTe share a lot of similarities with LaSbTe, and an additional CDW phase transition at 154 K is revealed in CeSbTe. However, the slower relaxation of CeSbTe exhibits an exotic behavior that deviates from the typical phonon-assisted electron-hole recombination process, probably due to the imbalance between the electron- and hole-type carriers. Unlike LaSbTe, the relaxation times of CeSbTe vary slightly with the pump power, inferring the possible participation of 4$f$ electron in the decay process. In addition, two oscillation modes around 1 THz and 3 THz are identified in both LaSbTe and CeSbTe, which are mostly likely to be coherent phonon modes. These findings unravel the existence of multiple CDW orders in LaSbTe and CeSbTe, offering insights into the underlying physics of these systems.

The spin Hall effect (SHE) allows efficient generation of spin polarization or spin current through charge current and plays a crucial role in the development of spintronics. While SHE typically occurs in non-magnetic materials and is time-reversal even, exploring time-reversal-odd (T-odd) SHE, which couples SHE to magnetization in ferromagnetic materials, offers a new charge-spin conversion mechanism with new functionalities. Here, we report the observation of giant T-odd SHE in Fe3GeTe2/MoTe2 van der Waals heterostructure, representing a previously unidentified interfacial magnetic spin Hall effect (interfacial-MSHE). Through rigorous symmetry analysis and theoretical calculations, we attribute the interfacial-MSHE to a symmetry-breaking induced spin current dipole at the vdW interface. Furthermore, we show that this linear effect can be used for implementing multiply-accumulate operations and binary convolutional neural networks with cascaded multi-terminal devices. Our findings uncover an interfacial T-odd charge-spin conversion mechanism with promising potential for energy-efficient in-memory computing.

The convergence of topology and correlations represents a highly coveted realm in the pursuit of novel quantum states of matter. Introducing electron correlations to a quantum spin Hall (QSH) insulator can lead to the emergence of a fractional topological insulator and other exotic time-reversal-symmetric topological order, not possible in quantum Hall and Chern insulator systems. However, the QSH insulator with quantized edge conductance remains rare, let alone that with significant correlations. In this work, we report a novel dual QSH insulator within the intrinsic monolayer crystal of TaIrTe4, arising from the interplay of its single-particle topology and density-tuned electron correlations. At charge neutrality, monolayer TaIrTe4 demonstrates the QSH insulator that aligns with single-particle band structure calculations, manifesting enhanced nonlocal transport and quantized helical edge conductance. Interestingly, upon introducing electrons from charge neutrality, TaIrTe4 only shows metallic behavior in a small range of charge densities but quickly goes into a new insulating state, entirely unexpected based on TaIrTe4's single-particle band structure. This insulating state could arise from a strong electronic instability near the van Hove singularities (VHS), likely leading to a charge density wave (CDW). Remarkably, within this correlated insulating gap, we observe a resurgence of the QSH state, marked by the revival of nonlocal transport and quantized helical edge conduction. Our observation of helical edge conduction in a CDW gap could bridge spin physics and charge orders. The discovery of a dual QSH insulator introduces a new method for creating topological flat minibands via CDW superlattices, which offer a promising platform for exploring time-reversal-symmetric fractional phases and electromagnetism., Comment: 23 pages, 15 figures, submitted version

The magnetism of Kitaev materials has been widely studied, but their charge properties and the coupling to other degrees of freedom are less known. Here we investigate the charge states of $\alpha$-RuCl$_3$, a promising Kitaev quantum spin liquid candidate, in proximity to graphite. We discover that few-layered $\alpha$-RuCl$_3$ experiences a clear modulation of charge states, where a Mott-insulator to weak charge-transfer-insulator transition in the 2D limit occurs by means of heterointerfacial polarization. More notably, distinct signals of incommensurate charge and lattice super-modulations, regarded as an unconventional charge order, accompanied in the insulator. Our theoretical calculations have reproduced the incommensurate charge order by taking into account the antiferroelectricity of $\alpha$-RuCl$_3$ that is driven by dipole order in the internal electric fields. The findings imply that there is strong coupling between the charge, spin, and lattice degrees of freedom in layered $\alpha$-RuCl$_3$ in the heterostructure, which offers an opportunity to electrically access and tune its magnetic interactions inside the Kitaev compounds., Comment: Accepted for publication in Nature Communications (20 pages, 4 figures)

Magnetic Weyl semimetal (MWS) is a unique topological state with open surface Fermi arc states and other exotic transport phenomena. However, most reported MWSs show multiple pairs of Weyl points and complicated Fermi surfaces, which increases the difficulty of the investigation into the intrinsic chiral transport property. In this wor, we successfully synthesized a soft magnetic Weyl semimetal Eu$_3$In$_2$As$_4$ with a single pair of Weyl points under magnetic fields. The Shubnikov de Haas (SdH) oscillation with a single frequency, as well as a linear hall resistance with the same carrier density, is observed up to 50 Tesla, indicating a single pair of Weyl points around the Fermi level with a massless fermion ($m^* = 0.121 m_0$, $\pi$ Berry phase). Such a single pair of Weyl points is further confirmed by the density functional theory calculations. The magnetic ordering and band topology can be easily tuned by the external magnetic field. The field-induced MWS Eu$_3$In$_2$As$_4$ with a single pair of Weyl points is a good platform to detect chiral transport properties, including possible quantum anomalous Hall effect.

The newly discovered Kagome superconductors AV$_3$Sb$_5$ (A=K, Rb and Cs) continue to bring surprises in generating unusual phenomena and physical properties, including anomalous Hall effect, unconventional charge density wave, electronic nematicity and time-reversal symmetry breaking. Here we report an unexpected emergence of multiple flat bands in the AV$_3$Sb$_5$ superconductors. By performing high-resolution angle-resolved photoemission (ARPES) measurements, we observed four branches of flat bands that span over the entire momentum space. The appearance of the flat bands is not anticipated from the band structure calculations and cannot be accounted for by the known mechanisms of flat band generation. It is intimately related to the evolution of van Hove singularities. It is for the first time to observe such emergence of multiple flat bands in solid materials. Our findings provide new insights in revealing the underlying mechanism that governs the unusual behaviors in the Kagome superconductors. They also provide a new pathway in producing flat bands and set a platform to study the flat bands related physics., Comment: 20 pages, 4 figures

Two-dimensional topological insulators (2DTIs) or quantum spin Hall insulators are attracting increasing attention due to their potential applications in next-generation spintronic devices. Despite their promising prospects, realizable 2DTIs are still limited. Recently, Ta2Pd3Te5, a semiconducting van der Waals material, has shown spectroscopic evidence of quantum spin Hall states. However, achieving controlled preparation of few- to monolayer samples, a crucial step in realizing quantum spin Hall devices, has not yet been achieved. In this work, we fabricated few- to monolayer Ta$_2$Pd$_3$Te$_5$ and performed systematic thickness- and temperature-dependent Raman spectroscopy measurements. Our results demonstrate that Raman spectra can provide valuable information to determine the thickness of Ta2Pd3Te5 thin flakes. Moreover, our angle-resolved polarized Raman (ARPR) spectroscopy measurements show that the intensities of the Raman peaks are strongly anisotropic due to the quasi-one-dimensional atomic structure, providing a straightforward method to determine its crystalline orientation. Our findings may stimulate further efforts to realize quantum devices based on few or monolayer Ta$_2$Pd$_3$Te$_5$.

Non-Hermitian physics, studying systems described by non-Hermitian Hamiltonians, reveals unique phenomena not present in Hermitian systems. Unlike Hermitian systems, non-Hermitian systems have complex eigenvalues, making their effects less directly observable. Recently, significant efforts have been devoted to incorporating the non-Hermitian effects into condensed matter physics. However, progress has been hindered by the absence of a viable experimental approach. Here, the discovery of surface-selectively spontaneous reconstructed Weyl semimetal NdAlSi provides a feasible experimental platform for studying non-Hermitian physics. Utilizing angle-resolved photoemission spectroscopy measurements, surface-projected density functional theory calculations, and scanning tunneling microscopy measurements, we demonstrate that surface reconstruction in NdAlSi alters surface Fermi arc connectivity and generates new isolated non-topological surface Fermi arcs. In the presence of a magnetic field, the surface-selective spontaneous reconstructed Weyl semimetal NdAlSi can be viewed as a Hermitian bulk--non-Hermitian boundary system. The isolated non-topological surface Fermi arcs on the reconstructed surface act as a loss mechanism and open boundary condition for the topological electrons and bulk states, serving as non-Hermitian boundary states. This discovery provides a good experimental platform for exploring new physical phenomena and potential applications based on boundary non-Hermitian effects, extending beyond purely mathematical concepts., Comment: 21 pages, 4 figures

For several decades, it was widely believed that a non-interacting disordered electronic system could only undergo an Anderson metal-insulator transition due to Anderson localization. However, numerous recent theoretical works have predicted the existence of a disorder-driven non-Anderson phase transition that differ from Anderson localization. The frustration lies in the fact that this non-Anderson disorder-driven transition has not yet been experimentally demonstrated in any system. Here, using angle-resolved photoemission spectroscopy, we present a case study of observing the non-Anderson disorder-driven transition by visualizing the electronic structure of the Weyl semimetal NdAlSi on surfaces with varying amounts of disorder. Our observations reveal that strong disorder can effectively suppress all surface states in the Weyl semimetal NdAlSi, including the topological surface Fermi arcs. This disappearance of surface Fermi arcs is associated with the vanishing of the bulk topological invariant, indicating a quantum phase transition from a Weyl semimetal to a diffusive metal. By analyzing the changes in the electronic structure of NdAlSi, as the surface degrades, we provide a physical picture of this non-Anderson transition from a Weyl semimetal to a diffuse metal. These observations provide the first direct experimental evidence of the non-Anderson disorder-driven transition, a discovery long anticipated by theoretical physicists. The finding dispels longstanding suspicions among researchers that non-Anderson transitions exist in real quantum systems., Comment: 13 pages, 4 figures

The excitonic insulator (EI) is an exotic ground state of narrow-gap semiconductors and semimetals arising from spontaneous condensation of electron-hole pairs bound by attractive Coulomb interaction. Despite research on EIs dating back to half a century ago, their existence in real materials remains a subject of ongoing debate. In this study, through systematic experimental and theoretical investigations, we provide evidence for the existence of an EI ground state in a van der Waals compound Ta$_2$Pd$_3$Te$_5$. Density-functional-theory calculations suggest that it is a semimetal with a small band overlap, whereas various experiments exhibit an insulating ground state with a clear band gap. Upon incorporating electron-hole Coulomb interaction into our calculations, we obtain an EI phase where the electronic symmetry breaking opens a many-body gap. Angle-resolved photoemission spectroscopy measurements exhibit that the band gap is closed with a significant change in the dispersions as the number of thermally excited charge carriers becomes sufficiently large in both equilibrium and nonequilibrium states. Structural measurements reveal a slight breaking of crystal symmetry with exceptionally small lattice distortion in the insulating state, which cannot account for the significant gap opening. Therefore, we attribute the insulating ground state with a gap opening in Ta$_2$Pd$_3$Te$_5$ to exciton condensation, where the coupling to the symmetry-breaking electronic state induces a subtle change in the crystal structure., Comment: 10 pages, 5 figures

The opening of an energy gap in the electronic structure generally indicates the presence of interactions. In materials with low carrier density and short screening length, long-range Coulomb interaction favors the spontaneous formation of electron-hole pairs, so-called excitons, opening an excitonic gap at the Fermi level. Excitonic materials host unique phenomenons associated with pair excitations. However, there is still no generally recognized single-crystal material with excitonic order, which is, therefore, awaited in condensed matter physics. Here, we show that excitonic states may exist in the quasi-one-dimensional material Ta$_2$Pd$_3$Te$_5$, which has an almost ideal Dirac-like band structure, with Dirac point located exactly at Fermi level. We find that an energy gap appears at 350 K, and it grows with decreasing temperature. The spontaneous gap opening is absent in a similar material Ta$_2$Ni$_3$Te$_5$. Intriguingly, the gap is destroyed by the potassium deposition on the crystal, likely due to extra-doped carriers. Furthermore, we observe a pair of in-gap flat bands, which is an analog of the impurity states in a superconducting gap. All these observations can be properly explained by an excitonic order, providing Ta$_2$Pd$_3$Te$_5$ as a new and promising candidate realizing excitonic states., Comment: 9 pages, 5 figures

Creating heterostructures with graphene/graphite is a practical method for charge-doping $\alpha$-RuCl$_3$, but not sufficient to cause the insulator-to-metal transition. In this study, detailed scanning tunneling microscopy/spectroscopy measurements on $\alpha$-RuCl$_3$ with various lattice deformations reveal that both in-plane and out-of-plane lattice distortions may collapse the Mott-gap in the case of monolayer $\alpha$-RuCl$_3$ in proximity to graphite, but have little impact on its bulk form alone. In the Mott-Hubbard framework, the transition is attributed to the lattice distortion-facilitated substantial modulation of the electron correlation parameter. Observation of the orbital textures on a highly compressed monolayer $\alpha$-RuCl$_3$ flake on graphite provides valuable evidence that electrons are efficiently transferred from the heterointerface into Cl3$p$ orbitals under the lattice distortion. It is believed that the splitting of Ru $t_{2g}$ bands within the trigonal distortion of Ru-Cl-Ru octahedra bonds generated the electrons transfer pathways. The increase of the Cl3$p$ states enhance the hopping integral in the Mott-Hubbard bands, resulting in the Mott-transition. These findings suggest a new route for implementing the insulator-to-metal transition upon doping in $\alpha$-RuCl$_3$ by deforming the lattice in addition to the formation of heterostructure., Comment: 9 pages, 5 figures, Accepted for publication in Physical Review B

Zirconium pentatelluride (ZrTe$_{5}$), a system with a Dirac linear band across the Fermi level and anomalous transport features, has attracted considerable research interest for it is predicted to be located at the boundary between strong and weak topological insulators separated by a topological semimetal phase. However, the experimental verification of the topological phase transition and the topological ground state in ZrTe$_{5}$ is full of controversies, mostly due to the difficulty of precisely capturing the small gap evolution with single-particle band structure measurements. Alternatively, the collective excitations of electric charges, known as plasmons, in Dirac systems exhibiting unique behavior, can well reflect the topological nature of the band structure. Here, using reflective high-resolution electron energy loss spectroscopy (HREELS), we investigate the temperature-dependent collective excitations of ZrTe$_{5}$, and discover that the plasmon energy in ZrTe$_{5}$ is proportional to the $1/3$ power of the carrier density $n$, which is a unique feature of plasmons in three-dimensional Dirac systems. Based on this conclusion, the origin of the resistivity anomaly of ZrTe$_{5}$ can be attributed to the temperature-dependent chemical potential shift in extrinsic Dirac semimetals., Comment: 7 pages, 4 figures

Quantum Spin Hall (QSH) insulators possess distinct helical in-gap states, enabling their edge states to act as one-dimensional conducting channels when backscattering is prohibited by time-reversal symmetry. However, it remains challenging to achieve high-performance combinations of nontrivial topological QSH states with superconductivity for applications and requires understanding of the complicated underlying mechanisms. Here, our experimental observations for a novel superconducting phase in the pressurized QSH insulator Ta2Pd3Te5 is reported, and the high-pressure phase maintains its original ambient pressure lattice symmetry up to 45 GPa. Our in-situ high-pressure synchrotron X-ray diffraction, electrical transport, infrared reflectance, and Raman spectroscopy measurements, in combination with rigorous theoretical calculations, provide compelling evidence for the association between the superconducting behavior and the abnormal densified phase. The isostructural transition was found to modify the topology of the Fermi surface directly, accompanied by a fivefold amplification of the density of states at 20 GPa compared to ambient pressure, which synergistically fosters the emergence of robust superconductivity. A profound comprehension of the fascinating properties exhibited by the compressed Ta2Pd3Te5 phase is achieved, highlighting the extraordinary potential of van der Waals (vdW) QSH insulators for exploring and investigating high-performance electronic advanced devices under extreme conditions., Comment: 16pages,4figures

Topological properties in quantum materials are often governed by symmetry and tuned by crystal structure and external fields, and hence symmetry-sensitive nonlinear optical measurements in a magnetic field are a valuable probe. Here we report nonlinear magneto-optical second harmonic generation (SHG) studies of non-magnetic topological materials including bilayer WTe2, monolayer WSe2 and bulk TaAs. The polarization-resolved patterns of optical SHG under magnetic field show nonlinear Kerr rotation in these time-reversal symmetric materials. For materials with three-fold rotational symmetric lattice structure, the SHG polarization pattern rotates just slightly in a magnetic field, whereas in those with mirror or two-fold rotational symmetry the SHG polarization pattern rotates greatly and distorts. These different magneto-SHG characters can be understood by considering the superposition of the magnetic field-induced time-noninvariant nonlinear optical tensor and the crystal-structure-based time-invariant counterpart. The situation is further clarified by scrutinizing the Faraday rotation, whose subtle interplay with crystal symmetry accounts for the diverse behavior of the extrinsic nonlinear Kerr rotation in different materials. Our work illustrates the application of magneto-SHG techniques to directly probe nontrivial topological properties, and underlines the importance of minimizing extrinsic nonlinear Kerr rotation in polarization-resolved magneto-optical studies., Comment: 25 pages, 6 figures

Finding viable Kagome lattices is vital for materializing novel phenomena in quantum materials. In this work, we performed element substitutions on CsV3Sb5 with space group P6/mmm, TbMn6Sn6 with space group P6/mmm, and CsV6Sb6 with space group R-3 m, respectively, as the parent compounds. A total of 4158 materials were obtained through element substitutions, and these materials were then calculated via density function theory in high-throughput mode. Afterward, 48 materials were identified with high thermodynamic stability (E_hull<5meV/atom). Furthermore, we compared the thermodynamic stability of three different phases with the same elemental composition and predicted some competing phases that may arise during material synthesis. Finally, by calculating the electronic structures of these materials, we attempted to identify patterns in the electronic structure variations as the elements change. This work provides guidance for discovering promising AM3X5/AM6X6 Kagome materials from a vast phase space.

Edge states in topological systems have attracted great interest due to their robustness and linear dispersions. Here a superconducting-proximitized edge interferometer is engineered on a topological insulator Ta2Pd3Te5 with asymmetric edges to realize the interfering Josephson diode effect (JDE), which hosts many advantages, such as the high efficiency as much as 73% at tiny applied magnetic fields with an ultra-low switching power around picowatt, and a giant interfering magnetochiral anisotropy with a maximal coefficient gamma = 1.2 x 10^{9} T^{-1}A^{-1}. As an important element to induce such JDE, the second-order harmonic in the current-phase relation is also experimentally confirmed by half-integer Shapiro steps. This edge interferometer offers a novel and effective method to enhance the overall performance of JDE and magnetochiral anisotropy, and boosts great potential applications for future superconducting quantum devices., Comment: 29 pages,21 figures

Magnetic kagome metals, in which topologically non-trivial band structures and electronic correlation are intertwined, have recently emerged as an exciting platform to explore exotic correlated topological phases, that are usually not found in weakly interacting materials described within the semi-classical picture of electrons. Here, via a comprehensive single-crystal neutron diffraction and first-principles density functional theory study of the archetypical topological kagome metal Mn$_3$Sn, which is also a magnetic Weyl fermion material and a promising chiral magnet for antiferromagnetic spintronics, we report the realisation of an emergent spin-density wave (SDW) order, a hallmark correlated many-body phenomenon, that is engineered by the Fermi surface nesting of topological flat bands. We further reveal that the phase transition, from the well-known high-temperature coplanar and non-collinear k = 0 inverse triangular antiferromagnetic order to a double-$k$ non-coplanar modulated incommensurate magnetic structure below $T_1$ = 280 K, is primarily driven by the SDW instability. The double-$k$ nature of this complex low-temperature magnetic order, which can be regarded as an intriguing superposition of a longitudinal SDW with a modulation wavevector k$_L$ and a transverse incommensurate helical magnetic order with a modulation wavevector k$_T$, is unambiguously confirmed by our observation of the inter-modulation high-order harmonics of the type of 2k$_L$+k$_T$. This discovery not only solves a long-standing puzzle concerning the nature of the phase transition at $T_1$, but also provides an extraordinary example on the intrinsic engineering of correlated many-body phenomena in topological matter. The identified multi-$k$ magnetic state can be further exploited for the engineering of the new modes of magnetization and chirality switching in antiferromagnetic spintronics.

Superconductivity in V-based kagome metals has recently raised great interest as they exhibit the competing ground states associated with the flat bands and topological electronic structures. Here we report the discovery of superconductivity in Ta2V3.1Si0.9 with a superconducting transition temperature Tc of 7.5 K, much higher than those in previously reported kagome metals at ambient pressure. While the V ions form a two-dimensional breathing kagome structure, the length difference between two different V-V bonds is just 0.04, making it very close to the perfect kagome structure. Our results show that Ta2V3.1Si0.9 is a moderate-coupled superconductor with a large upper critical field that is close to the Pauli limit. DFT calculations give a van-Hove-singularity band located at Fermi energy, which may explain the relatively high Tc observed in this material., Comment: 24 pages, 6 figures

Emergent phases often appear when the electronic kinetic energy is comparable to the Coulomb interactions. One approach to seek material systems as hosts of such emergent phases is to realize localization of electronic wavefunctions due to the geometric frustration inherent in the crystal structure, resulting in flat electronic bands. Recently, such efforts have found a wide range of exotic phases in the two-dimensional kagome lattice, including magnetic order, time-reversal symmetry breaking charge order, nematicity, and superconductivity. However, the interlayer coupling of the kagome layers disrupts the destructive interference needed to completely quench the kinetic energy. Here we demonstrate that an interwoven kagome network-a pyrochlore lattice-can host a three dimensional (3D) localization of electron wavefunctions. Meanwhile, the nonsymmorphic symmetry of the pyrochlore lattice guarantees all band crossings at the Brillouin zone X point to be 3D gapless Dirac points, which was predicted theoretically but never yet observed experimentally. Through a combination of angle-resolved photoemission spectroscopy, fundamental lattice model and density functional theory calculations, we investigate the novel electronic structure of a Laves phase superconductor with a pyrochlore sublattice, CeRu$_2$. We observe flat bands originating from both the Ce 4$f$ orbitals as well as from the 3D destructive interference of the Ru 4$d$ orbitals. We further observe the nonsymmorphic symmetry-protected 3D gapless Dirac cones at the X point. Our work establishes the pyrochlore structure as a promising lattice platform to realize and tune novel emergent phases intertwining topology and many-body interactions., Comment: 27 pages, 4 figures

The study of interaction between electromagnetism and elementary particles is a long-standing topic in physics. Likewise, the connection between particle physics and emergent phenomena in condensed matter physics is a recurring theme and condensed matter physics has often provided a platform for investigating the interplay between particles and fields in cases that have not been observed in high-energy physics, so far. Here, using angle-resolved photoemission spectroscopy, we provide a new example of this by visualizing the electronic structure of a noncentrosymmetric magnetic Weyl semimetal candidate NdAlSi in both the paramagnetic and ferrimagnetic states. We observe surface Fermi arcs and bulk Weyl fermion dispersion as well as the regulation of Weyl fermions by ferrimagnetism. Our results establish NdAlSi as a magnetic Weyl semimetal and provide the first experimental observation of ferrimagnetic regulation of Weyl fermions in condensed matter., Comment: 19 pages, 4 figures

The discovery of the topological states has become a key topic in condensed matter physics with the focus evolving from the Dirac or Weyl points to high-dimension topological states of the nodal lines and nodal surfaces. For a topological material to manifest its quantum properties and become useful in applications, the topological states need to be genuine and clean so that they lie close to the Fermi level without other trivial bands existing at the Fermi level. While a number of high-dimension topological materials are predicted, only a few of them have been synthesized and confirmed and the genuine and clean ones are especially scarce. Here we report the realization of the genuine clean multiple high-dimension topological states in NaAlSi. By performing high-resolution angle-resolved photoemission measurements and band structure calculations, we have observed two sets of nodal surfaces and the formation of two homocentric nodal ring states in NaAlSi. The observed nodal rings are distinct in that the inner one is a type-{\uppercase\expandafter{\romannumeral1}} nodal ring while the outer one is a type-{\uppercase\expandafter{\romannumeral1}} nodal ring embedded with four type-{\uppercase\expandafter{\romannumeral3}} nodal points. All the bands involved in the nodal rings lie very close to the Fermi level with no other trivial bands coexisting at the Fermi level. These observations make NaAlSi a desirable topological material to explore for novel quantum states and exotic properties.

The superconductor SnTaS$_{2}$ is theoretically predicted to be an intriguing topological nodal line semimetal without consideration of spin-orbit coupling. By carrying out angle-resolved photoemission (ARPES) and spin-resolved ARPES measurements combined with band structure calculations, we have provided a complete picture of the electronic structure and spin polarization property for the prominent surface states of SnTaS$_{2}$. The low-energy electronic states are dominated by surface states; two of them are from the S-terminated surface, while four of them are from the Sn-terminated surface. These give rise to interesting Fermi surface topology of SnTaS$_{2}$: three pockets located at $\bar\Gamma$, $\bar{M}$ and $\bar{K}$ for the S-terminated surface and two pockets surrounding $\bar\Gamma$ and $\bar{K}$ for the Sn-terminated surface. We further reveal that two surface states that cross the Fermi level are spin-polarized. Since SnTaS$_{2}$ is also a superconductor, our observations indicate that it may provide a new platform to explore topological superconductivity and other exotic properties.

In the ferrimagnetic nodal-line semiconductor Mn$_3$Si$_2$Te$_6$, colossal magnetoresistance (CMR) arises below $T_\mathrm{c}=78$ K due to the interplay of magnetism and topological nodal-line fermiology. The Berry curvature associated with the topological nodal-line is expected to produce an anomalous Nernst effect. Here, we present sizable anomalous Nernst signal in Mn$_3$Si$_2$Te$_6$ below $T_\mathrm{c}$. In the low-magnetic-field region where CMR is most apparent, the scaling ratio between the Nernst signal and magnetization is significantly enhanced compared to that in conventional magnetic materials. The enhanced Nernst effect and CMR likely share the same mechanisms, which are closely linked to the nodal-line topology., Comment: 6 pages, 4 figures

Quantum magneto-oscillations have long been a vital subject in condensed matter physics, with ubiquitous quantum phenomena and diverse underlying physical mechanisms. Here, we demonstrate the intrinsic and reproducible DC-current-driven quantum electro-oscillations with a periodicity in the inverse of the current (1/I), in quasi-one-dimensional charge-density-wave (CDW) insulators (TaSe$_4$)$_2$I and TaS$_3$ nanowires. Such oscillations manifest in the nearly infinite Fr\"ohlich conductivity region where the undamped CDW flow forms in a finite electric current, and finally disappear after the oscillation index n reaches 1. A systematic investigation on the effect of temperature and magnetic field establishes that the observed electro-oscillations are a coherent quantum phenomenon. We discuss the possibilities of the physical mechanisms, including the formation of sliding-driven inherent Floquet sidebands. Our results introduce a new member in the family of quantum oscillations, and shed light on plausible avenues to explore novel physics and potential applications of coherent density-wave condensates., Comment: 33 pages, 17 figures

The energy spectrum of topological semimetals contains protected degeneracies in reciprocal space that correspond to Weyl, Dirac, or multifold fermionic states. To exploit the unconventional properties of these states, one has to access the electronic structure of the three-dimensional bulk. In this work, we resolve the bulk electronic states of candidate topological semimetal FeSi using momentum-dependent resonant inelastic X-ray scattering (RIXS) at the Fe $L_3$ edge. We observe a broad excitation continuum devoid of sharp features, consistent with particle-hole scattering in an underlying electronic band structure. Using density functional theory, we calculate the electronic structure of FeSi and derive a band theory formulation of RIXS in the fast collision approximation to model the scattering process. We find that band theory qualitatively captures the number and position of the main spectral features, as well as the overall momentum dependence of the RIXS intensity. Our work paves the way for targeted studies of band touchings in topological semimetals with RIXS.

TaAs, the first experimentally discovered Weyl semimetal material, has attracted a lot of attention due to its high carrier mobility, high anisotropy, nonmagnetic and strong interaction with light. These make it an ideal candidate for the study of Weyl fermions and the applications in quantum computation, thermoelectric devices, and photodetection. For further basic physics studies and potential applications, large-size and high-quality TaAs films are urgently needed. However, it is difficult to grow As-stoichiometry TaAs films due to the volatilization of As during the growth. To solve this problem, the TaAs films were attempted to grow on different substrates using targets with different As stoichiometric ratios by pulsed laser deposition (PLD). In this work, we have found that partial As ions of the GaAs substrate are likely to diffuse into the TaAs films during growth, which was preliminarily confirmed by the structural characterization, surface topography and composition analysis. As a result, the As content in the TaAs film is improved and the TaAs phase is achieved. Our work presents an effective method to fabricate the TaAs films by PLD, providing the possible use of the Weyl semimetal film for functional devices.

Recently, the hexagonal phase of ternary transition metal pnictides TT'X (T = Zr, Hf; T'= Ru; X = P, As), which are well-known noncentrosymmetric superconductors, were predicted to host nontrivial bulk topology. In this work, we systematically investigate the electronic responses of ZrRuAs to external pressure. At ambient pressure, ZrRuAs show superconductivity with Tc ~ 7.74 K, while a large upper critical field ~ 13.03 T is obtained for ZrRuAs, which is comparable to the weak-coupling Pauli limit. The resistivity of ZrRuAs exhibits a non-monotonic evolution with increasing pressure. The superconducting transition temperature Tc increases with applied pressure and reaches a maximum value of 7.93 K at 2.1 GPa, followed by a decrease. The nontrivial topology is robust and persists up to the high-pressure regime. Considering both robust superconductivity and intriguing topology in this material, our results could contribute to studies of the interplay between topological electronic states and superconductivity., Comment: 17 pages,6 figures, 1 table

The building block of in-memory computing with spintronic devices is mainly based on the magnetic tunnel junction with perpendicular interfacial anisotropy (p-MTJ). The resulting asymmetric write and read-out operations impose challenges in downscaling and direct cascadability of p-MTJ devices. Here, we propose that a new symmetric write and read-out mechanism can be realized in perpendicular-anisotropy spin-orbit (PASO) quantum materials based on Fe3GeTe2 and WTe2. We demonstrate that field-free and deterministic reversal of the perpendicular magnetization can be achieved by employing unconventional charge to z-spin conversion. The resulting magnetic state can be readily probed with its intrinsic inverse process, i.e., z-spin to charge conversion. Using the PASO quantum material as a fundamental building block, we implement the functionally complete set of logic-in-memory operations and a more complex nonvolatile half-adder logic function. Our work highlights the potential of PASO quantum materials for the development of scalable energy-efficient and ultrafast spintronic computing., Comment: Accepted by Science Advances

Recent discovery of topologically non-trivial behavior in Co3Sn2S2 stimulated a notable interest in this itinerant ferromagnet (Tc = 174 K). The exact magnetic state remains ambiguous, with several reports indicating the existence of a second transition in the range 125 -- 130 K, with antiferromagnetic and glassy phases proposed to coexist with the ferromagnetic phase. Using detailed angle-dependent DC and AC magnetization measurements on large, high-quality single crystals we reveal a highly anisotropic behavior of both static and dynamic response of Co3Sn2S2. It is established that many observations related to sharp magnetization changes when B || c are influenced by the demagnetization factor of a sample. On the other hand, a genuine transition has been found at Tp = 128 K, with the magnetic response being strictly perpendicular to the c-axis and several orders of magnitude smaller than for B || c. Calculations using density-functional theory indicate that the ground state magnetic structure consist of magnetic moments canted away from the c-axis by a small angle (~ 1.5deg). We argue that the second transition originates from a small additional canting of moments within the kagome plane, with two equivalent orientations for each spin., Comment: accepted as a Letter in PRB

1T-TiSe2 is one of the most studied charge density wave (CDW) systems, not only because of its peculiar properties related to the CDW transition, but also due to its status as a promising candidate of exciton insulator signaled by the proposed plasmon softening at the CDW wave vector. Using high-resolution electron energy loss spectroscopy, we report a systematic study of the temperature-dependent plasmon behaviors of 1T-TiSe2. We unambiguously resolve the plasmon from phonon modes, revealing the existence of Landau damping to the plasmon at finite momentums, which does not support the plasmon softening picture for exciton condensation. Moreover, we discover that the plasmon lifetime at zero momentum responds dramatically to the bandgap evolution associated with the CDW transition. The interband transitions near the Fermi energy in the normal phase is demonstrated serving as a strong damping channel of plasmons, while such a channel in the CDW phase is suppressed due to the CDW gap opening, which results in the dramatic tunability of the plasmon in semimetals or small-gap semiconductors.

All van der Waals (vdW) Fe3GeTe2/Cr2Ge2Te6/graphite magnetic heterojunctions have been fabricated via mechanical exfoliation and stacking, and their magnetotransport properties are studied in detail. At low bias voltages large negative junction magnetoresistances have been observed and are attributed to spin-conserving tunneling transport across the insulating Cr2Ge2Te6 layer. With increasing bias, a crossover to Fowler-Nordheim tunneling takes place. The negative sign of the tunneling magnetoresistance (TMR) suggests that the bottom of conduction band in Cr2Ge2Te6 belongs to minority spins, opposite to the findings of some first-principles calculations. This work shows that the vdW heterostructures based on 2D magnetic insulators are a valuable platform to gain further insight into spin polarized tunneling transport, which is the basis for pursuing high performance spintronic devices and a large variety of quantum phenomena., Comment: 17 pages, 4 figures. This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing

The interplay between topology and interaction always plays an important role in condensed matter physics and induces many exotic quantum phases, while rare transition metal layered material (TMLM) has been proved to possess both. Here we report a TMLM Ta$_2$Pd$_3$Te$_5$ has the two-dimensional second-order topology (also a quadrupole topological insulator) with correlated edge states - Luttinger liquid. It is ascribed to the unconventional nature of the mismatch between charge- and atomic- centers induced by a remarkable double-band inversion. This one-dimensional protected edge state preserves the Luttinger liquid behavior with robustness and universality in scale from micro- to macro- size, leading to a significant anisotropic electrical transport through two-dimensional sides of bulk materials. Moreover, the bulk gap can be modulated by the thickness, resulting in an extensive-range phase diagram for Luttinger liquid. These provide an attractive model to study the interaction and quantum phases in correlated topological systems., Comment: 41 pages, 6 Main Figures + 14 Supplementary Figure

The electronic structure and the physical properties of quantum materials can be significantly altered by charge carrier doping and magnetic state transition. Here we report a discovery of a giant and reversible electronic structure evolution with doping in a magnetic topological material. By performing high-resolution angle-resolved photoemission measurements on EuCd2As2,we found that a huge amount of hole doping can be introduced into the sample surface due to surface absorption. The electronic structure exhibits a dramatic change with the hole doping which can not be described by a rigid band shift. Prominent band splitting is observed at high doping which corresponds to a doping-induced magnetic transition at low temperature (below -15 K) from an antiferromagnetic state to a ferromagnetic state. These results have established a detailed electronic phase diagram of EuCd2As2 where the electronic structure and the magnetic structure change systematically and dramatically with the doping level. They further suggest that the transport, magnetic and topological properties of EuCd2As2 can be greatly modified by doping. These work will stimulate further investigations to explore for new phenomena and properties in doping this magnetic topological material., Comment: 22 pages,5 figures

Topological insulators with intrinsic magnetic order are emerging as an exciting platform to realize fundamentally new excitations from topological quantum states of matter. To study these systems and their physics, people have proposed a variety of magnetic topological insulator systems, including HoSbTe, an antiferromagnetic weak topological insulator candidate. In this work, we use scanning tunneling microscopy to probe the electronic structure of HoSbTe with antiferromagnetic and ferromagnetic orders that are tuned by applying an external magnetic field. Although around the Fermi energy, we find minor differences between the quasi-particle interferences under the ferromagnetic and antiferromagnetic orders, deep inside the valance region, a new quasi-particle interference signal emerges with ferromagnetism. This observation is consistent with our first-principles calculations indicating the magnetism-driven transition of the electronic states in this spin-orbit coupled topological magnet., Comment: 13 pages, 7 figures

The fabrication of one-dimensional (1D) magnetic systems on solid surfaces, although of high fundamental interest, has yet to be achieved for a crossover between two-dimensional (2D) magnetic layers and their associated 1D spin chain systems. In this study, we report the fabrication of 1D single-unit-cell-width CrCl3 atomic wires and their stacked few-wire arrays on the surface of a van der Waals (vdW) superconductor NbSe2. Scanning tunneling microscopy/spectroscopy and first-principles calculations jointly revealed that the single wire shows an antiferromagnetic large-bandgap semiconducting state in an unexplored structure different from the well-known 2D CrCl3 phase. Competition among the total energies and nanostructure-substrate interfacial interactions of these two phases result in the appearance of the 1D phase. This phase was transformable to the 2D phase either prior to or after the growth for in situ or ex situ manipulations, in which the electronic interactions at the vdW interface play a nontrivial role that could regulate the dimensionality conversion and structural transformation between the 1D-2D CrCl3 phases., Comment: 4 figures