Abstract Magnetically intercalated transition metal dichalcogenides are emerging as a rich platform for exploring exotic quantum states in van der Waals magnets. Among them, Co x TaS2 has attracted intense interest following the recent discovery of a distinctive 3Q magnetic ground state and a pronounced topological Hall effect below a critical doping of x ≈ 1/3, both intimately tied to cobalt concentration. To date, direct signatures of this enigmatic 3Q magnetic order in the electronic structure remain elusive. Here we report a comprehensive doping dependent angle resolved photoemission spectroscopy study that unveils these long-sought fingerprints. Our data reveal an unexpected inverse-Mexican-hat dispersion along the K-M- $${\mathrm{K}}^{\prime}$$ K ′ direction, accompanied by two van Hove singularities. These features are consistent with theoretical predictions for a 3Q magnetic order near three-quarters band filling on a cobalt triangular lattice. These results provide evidence of 3Q magnetic order in the electronic structure, establishing TMD van der Waals magnets as tunable materials to explore the interplay between magnetism and topology.
Topological Dirac materials are characterized by linear band crossings near the Fermi level, giving rise to quasiparticles that behave as massless Dirac fermions. In layered transition-metal dichalcogenides (TMDCs), such states arise within a symmetry-rich and structurally versatile material platform. Angle-resolved photoemission spectroscopy (ARPES) directly probes the momentum-resolved electronic band structure, making it a key tool for identifying Dirac dispersions and topological band features. This mini-review focuses on recent ARPES studies of topological Dirac electronic states in group-10 tellurides and vanadium based TMDCs. We highlight experimental observations of Dirac dispersions and their evolution under external perturbations such as composition tuning, strain, and thickness control. Furthermore, we discuss how spin-orbit coupling and electron correlation reshape the Dirac band structure. Through these ARPES-based findings, we aim to provide an updated perspective on topological band engineering in TMDCs and their relevance to quantum material research.
Van der Waals materials enable the construction of atomically sharp interfaces between compounds with distinct crystal and electronic properties. This is dramatically exploited in moiré systems, where a lattice mismatch or twist between monolayers generates an emergent in-plane periodicity, giving rise to electronic properties absent in the constituent materials. In contrast, vertical superlattices, formed by stacking dissimilar materials in the out-of-plane direction on the nanometer scale, have received far less attention despite their potential to realize analogous emergent phenomena in three dimensions. Through angle-resolved photoemission spectroscopy and density functional theory, we investigate six-to-eight-layer transition metal dichalcogenide (TMD) heterostructures constructed from pairs of stacked few-layer materials. Counterintuitively, we find that even these single superlattice units can host fully delocalized bands, evidencing a robust coherent interlayer coupling across lattice-mismatched interfaces over extended spatial scales. We show how uncompensated semimetallic phases and energetically mismatched topological surface states are readily and exclusively stabilized within such asymmetrical architectures. These findings establish two-component heterostructures in the intermediate-layer regime as platforms to invoke and control unprecedented combinations and instances of the diverse quantum phases native to many-layer TMDs.
The spin and orbital angular momentum (SAM and OAM) are conceptually analogous, yet their roles in condensed matter systems have not been often treated on equal footing. While SAM has been extensively explored, OAM has long been regarded as quenched in crystalline environments and thus largely overlooked. Recent experimental and theoretical advances, however, have demonstrated that OAM can drive a variety of novel electronic phenomena, highlighting the importance of probing OAM textures in the electronic band structure. Here, we investigate the momentum-space OAM texture of (TaSe4)2I, a one-dimensional chiral crystal. Using circular-dichroism angle-resolved photoemission spectroscopy (CD-ARPES), we uncover a p-wave OAM texture accompanied by OAM dipole structures. This orbital p-wave texture is intimately connected to, and thus controllable by the chirality of the host lattice. Complementary spin-resolved ARPES measurements and first-principles calculations reveal that the OAM polarization overwhelmingly dominates the low-energy electronic properties of (TaSe4)2I, far exceeding the SAM polarization. These observations represent the experimental verification of a new type of OAM texture in crystalline materials. Most importantly, these findings underscore a promising material platform for spinless orbitronics applications and lay the foundation for realizing multipolar OAM textures-orbital counterparts of the spin texture in unconventional magnets.
The checkerboard lattice has been proposed to host topological flat bands as a result of destructive interference among its various electronic hopping terms. However, it has proven challenging to realize experimentally due to the difficulty of isolating this structure from any significant out-of-plane bonding while maintaining structural integrity. Here, single crystals of Zr2CuSb3, a potential candidate for the checkerboard lattice, were synthesized using the solution (self-flux) method, and their structure was confirmed via x-ray diffraction. Electrical-transport measurements indicate metallic behavior with electron-dominated carriers. Angle-resolved photoemission spectroscopy reveals multiple electron pockets and significant kz broadening due to its large c axis and low dispersion features in kz. Density-functional theory (DFT) calculations further disentangle the contributions from each high-symmetry plane, providing a comprehensive characterization of electronic behavior. The DFT calculations were then used to determine the orbital contributions of the bands and detect the out-of-plane bonding which prevented the flat bands from forming.
The pursuit of emergent quantum phenomena lies at the forefront of modern condensed matter physics. A recent breakthrough in this arena is the discovery of the fractional quantum anomalous Hall effect (FQAHE) in twisted bilayer MoTe₂ (tbMoTe₂), marking a paradigm shift and establishing a versatile platform for exploring the intricate interplay among topology, magnetism, and electron correlations. While significant progress has been made through both optical and electrical transport measurements, direct experimental insights into the electronic structure – crucial for understanding and modeling this system – have remained elusive. Here, using spatially and angle-resolved photoemission spectroscopy (μ-ARPES), we directly map the electronic band structure of tbMoTe₂. We identify the valence band maximum, whose partial filling underlies the FQAHE, at the K points, situated approximately 150 meV above the Γ valley. By fine-tuning the doping level via in-situ alkali metal deposition, we also resolve the conduction band minimum at the K point, providing direct evidence that tbMoTe₂ exhibits a direct band gap – distinct from all previously known moiré bilayer transition metal dichalcogenide systems. These results offer critical insights for theoretical modeling and advance our understanding of fractionalized excitations and correlated topological phases in this emergent quantum material. Twisted bilayer (tb) MoTe2 is an ideal platform for investigating the fractional quantum anomalous Hall effect but issues related to air sensitivity make the study of its electronic structure experimentally challenging. As a solution, the authors prepare hBN encapsulated tb-MoTe2 and using micro-angle resolved photoemission spectroscopy determine the band structure. Furthermore, through in-situ alkali metal deposition, they obtain evidence indicating a direct band gap.
Advances in chemical vapor deposition (CVD) growth have driven graphene crystal quality to unprecedented levels, yet it is still unknown whether this route can realize the fragile flat-band and correlated states of the magic-angle (MA) twisted bilayer graphene (TBG). Here, we report on the experimental observation by room-temperature nano-angle-resolved photoemission spectroscopy (nano-ARPES) of flat bands in a TBG sample close to the MA, assembled via a grow-and-stack protocol based on low-pressure CVD of graphene on copper. Our study indicates electronic bands fully comparable to those measured in exfoliation-based samples and determines the size of the largest near-MA domain to be compatible with electronic transport experiments, motivating further experiments on flat-band physics in CVD-graphene.
CsGeX3, a class of halide perovskites, is an emergent semiconductor with ferroelectricity and potential optoelectronic properties that can be harnessed for device applications. However, measurements of the electronic structure for this class of material are still lacking. In this work, we report, for the first time, the experimental band structures of CsGeI3, a ferroelectric halide perovskite semiconductor, through angle-resolved photoemission spectroscopy (ARPES). The crystals were cleaved along both the (110) and (111) surfaces, facilitating the observation of clear valence band dispersions in several high-symmetry momentum directions. The observed valence band is characterized by a small hole effective mass of similar to 0.1m 0 at the valence band maximum, without notable spectral signatures associated with the Rashba effect. Our experimental measurements are supported by electronic structure calculations in the DFT + G0W0 framework, enabling assessment of the band orbital characteristics, dispersion, and spin-splitting. This work unveils the intrinsic electronic and transport properties of CsGeX3, thereby advancing the optimization of the optoelectronic properties of this class of materials.
Discovering and engineering spin-polarized surface states in the electronic structures of condensed matter systems is a crucial first step in the development of spintronic devices, wherein spin-polarized bands crossing the Fermi level can facilitate information transfer. Here, through nanofocused angle-resolved photoemission spectroscopy (nano-ARPES) and density functional theory-based calculations, we show that the interface between monolayer WSe2 and metallic NbSe2 exhibits a negative Schottky barrier height of ∼ -30 meV: the K-point valleys of the semiconducting layer are shifted by ∼800 meV to produce a surface-localized Fermi surface populated only by spin-polarized charge carriers. By increasing the WSe2 thickness, the Fermi pockets can be moved from K to Γ, demonstrating tunability of novel semimetallic phases that exist atop a substrate additionally possessing charge density wave and superconducting phases. Together, this study provides a spectroscopic understanding into p-type, Schottky barrier-free interfaces, which are of urgent interest for bypassing the limitations of current-generation vertical field effect transistors, in addition to longer-term spintronics development.
Electron-boson coupling is central to a comprehensive understanding of the diverse physical phenomena emerging from many-body interactions. Yet less attention has been paid to how plasmons, collective bosonic modes of electron density oscillation, interact with conduction electrons and how external parameters can tune this interaction. Here, we present a clear display of composite quasiparticles stemming from electron-plasmon coupling, known as the plasmonic polaron, in self-intercalated 1T-TiS2, by using angle-resolved photoemission spectroscopy (ARPES), high-resolution electron energy loss spectroscopy (HR-EELS) and first-principles calculations. The single particle spectral function exhibits a distinctive plasmon-loss satellite with the same characteristic energy scale determined by HR-EELS measurements. The bosonic energy scale of plasmonic polaron is tunable by controlling charge carrier density and temperature, distinguishing itself from conventional polarons arising from electron-phonon interactions. Furthermore, we find that the dielectric screening strongly affects the formation of the plasmonic polaron states. Our findings provide direct spectroscopic evidence of plasmonic polarons and establish self-intercalated layered materials as a promising platform for studying, controlling, and harnessing plasmonic interactions in quantum materials.
Vacuum ultraviolet photoemission spectroscopies are very information-rich experiments, but due to their surface sensitivity, data are often collected on an initially uncharacterized surface. Traditional raster-grid approaches for locating optimal measurement regions can be time-consuming. In this work, we introduce AARDVARK, a generalizable framework for sample exploration that leverages dimensionality reduction and Gaussian process regression to guide initial sample searches in spatially-resolved photoemission experiments. By utilizing UMAP as a target for a Gaussian process, the algorithm efficiently identifies boundaries of spectroscopically distinct regions, dynamically adapting to variations in sample characteristics. The algorithm enables real-time decision making in measurement selection, optimizes data acquisition, and presents a robust framework for future autonomous sample exploration in photoemission experiments.
The symmetry-broken correlated states in twisted double bilayer graphene (TDBG) can be tuned via several external knobs, including twist angle, displacement field, and carrier density. However, a direct, momentum-resolved characterization of how these parameters reshape the flat-band structure remains limited. In this Letter, we employ microfocused angle-resolved photoemission spectroscopy to investigate the flat-band dispersion of TDBG at a twist angle of 1.6 degrees, systematically varying the displacement field and carrier density via electrostatic gating. We directly observe multiple flat moire minibands near charge neutrality, including a flat remote valence band residing below the low-energy flat-band manifold. Furthermore, the dominant Coulomb repulsive energy over the flat-band bandwidth suggests favorable conditions for the emergence of interaction-driven correlated phenomena in TDBG. These findings establish that the formation and evolution of flat bands in TDBG arises from the interplay between the electron filling and the displacement field.
Tuning and probing spin-valley coupling is key to understanding correlated ground states in 2H-TaS2. Its magnetically intercalated analogue, Co1/3TaS2, introduces additional degrees of freedom, including modified interlayer coupling and magnetism, to modulate spin-valley physics. Surface-sensitive probes like ARPES are essential for accessing surface spin texture, yet previous studies on 2H-TMDs have reported conflicting results regarding spin-polarized bands, leaving open whether these discrepancies are intrinsic or extrinsic. Here we performed spatially resolved spin-ARPES measurements on 2H-TaS2 and Co1/3TaS2. Our results reveal robust spin-valley locking on both compounds. Importantly, Co intercalation enhances interlayer hybridization and introduces magnetism while preserving the TaS2-derived spin texture. We further observe a spatial reversal of the out-of-plane spin polarization, which we attribute to different surface domains. This effect complicates quantifying spin textures and may underlie prior inconsistent observations. Our findings provide microscopic insight into how interlayer interactions and surface domains together govern spin-valley phenomena in layered TMDs.
Tomonaga-Luttinger liquid (TLL) behavior in one-dimensional systems has been predicted and shown to occur at semiconductor-to-metal transitions within two-dimensional materials. Reports of one-dimensional defects hosting a Fermi liquid or a TLL have suggested a dependence on the underlying substrate, however, unveiling the physical details of electronic contributions from the substrate require cross-correlative investigation. Here, we study TLL formation within defectively engineered WS_2 atop graphene, where band structure and the atomic environment is visualized with nano angle-resolved photoelectron spectroscopy, scanning tunneling microscopy and spectroscopy, and non-contact atomic force microscopy. Correlations between the local density of states and electronic band dispersion elucidated the electron transfer from graphene into a TLL hosted by one-dimensional metal (1DM) defects. It appears that the vertical heterostructure with graphene and the induced charge transfer from graphene into the 1DM is critical for the formation of a TLL.
Non-magnetic FeNb_3Se_10 has been demonstrated to be an insulator at ambient pressure through both theoretical calculations and experimental measurements and it does not host topological surface states. Here we show that on the application of pressure, FeNb_3Se_10 transitions to a metallic state at around 3.0 GPa. With a further increase in pressure, its resistivity becomes independent of both temperature and pressure. Its crystal structure is maintained to at least 4.4 GPa.
Layered nickelates have been studied extensively over the last three decades due to their structural similarities to the high-${T}_{c}$ superconducting cuprates. Using reactive oxide molecular beam epitaxy (MBE), we synthesize ${\mathrm{Nd}}_{2\ensuremath{-}x}{\mathrm{Sr}}_{x}{\mathrm{NiO}}_{4}$ thin films for $x=0\ensuremath{-}1.4$ to probe the properties and electronic structure as a function of hole doping. The samples with lower doping show semiconducting behavior across the temperatures probed with an onset of metallic conductivity at $x=1.4$. We also present polarization-dependent O $K$ and Ni ${L}_{2,3}$ x-ray absorption spectra to track the evolution of the oxygen-nickel hybridization, distribution of holes between O $2p$ and Ni $3d$ states and the nickel oxidation state across the series. Angle-resolved photoemission spectroscopy (ARPES) measurements reveal a Fermi surface that comprises a cupratelike hole pocket of ${d}_{{x}^{2}\ensuremath{-}{y}^{2}}$ character with an additional electron pocket of ${d}_{3{z}^{2}\ensuremath{-}{r}^{2}}$ character at $\mathrm{\ensuremath{\Gamma}}$. The emergence of a quasiparticle peak at the Fermi vector for $x=1.4$ corroborates the insulator-to-metal transition at $x\ensuremath{\sim}1$. Finally, observe a fully two-dimensional Fermi surface with no momentum-dependent pseudogap, in contrast to measurements of the related bulk compound, ${\mathrm{Eu}}_{0.9}{\mathrm{Sr}}_{1.1}{\mathrm{NiO}}_{4}$.
The quantum metric tensor is a central geometric quantity in modern physics that is defined as the distance between nearby quantum states. Despite numerous studies highlighting its relevance to fundamental physical phenomena in solids, measuring the complete quantum metric tensors in real solid-state materials is challenging. In this work, we report a direct measurement of the full quantum metric tensors of Bloch electrons in solids using black phosphorus as a representative material. We extracted the momentum space distribution of the pseudospin texture of the valence band from the polarization dependence of angle-resolved photoemission spectroscopy measurement. Our approach is poised to advance our understanding of quantum geometric responses in a wide class of crystalline systems.