Spin-orbit coupling in noncentrosymmetric crystals leads to spin-momentum locking - a directional relationship between an electron's spin angular momentum and its linear momentum. Isotropic orthogonal Rashba spin-momentum locking has been studied for decades, while its counterpart, isotropic parallel Weyl spin-momentum locking has remained elusive in experiments. Theory predicts that Weyl spin-momentum locking can only be realized in structurally chiral cubic crystals in the vicinity of Kramers-Weyl or multifold fermions. Here, we use spin- and angle-resolved photoemission spectroscopy to evidence Weyl spin-momentum locking of multifold fermions in the chiral topological semimetal PtGa. We find that the electron spin of the Fermi arc surface states is orthogonal to their Fermi surface contour for momenta close to the projection of the bulk multifold fermion at the Γ point, which is consistent with Weyl spin-momentum locking of the latter. The direct measurement of the bulk spin texture of the multifold fermion at the R point also displays Weyl spin-momentum locking. The discovery of Weyl spin-momentum locking may lead to energy-efficient memory devices and Josephson diodes based on chiral topological semimetals.
The currently established electronic phase diagram of cuprates is based on a study of single- and double-layered compounds. These CuO2 planes, however, are directly contacted with dopant layers, thus inevitably disordered with an inhomogeneous electronic state. Here, we solve this issue by investigating a 6-layered Ba2Ca5Cu6O12(F,O)2 with inner CuO2 layers, which are clean with the extremely low disorder, by angle-resolved photoemission spectroscopy (ARPES) and quantum oscillation measurements. We find a tiny Fermi pocket with a doping level less than 1% to exhibit well-defined quasiparticle peaks which surprisingly lack the polaronic feature. This provides the first evidence that the slightest amount of carriers is enough to turn a Mott insulating state into a metallic state with long-lived quasiparticles. By tuning hole carriers, we also find an unexpected phase transition from the superconducting to metallic states at 4%. Our results are distinct from the nodal liquid state with polaronic features proposed as an anomaly of the heavily underdoped cuprates.
Copper , Superconductivity , Electronics , Phase Transition
We report the evolution of the electronic structure at the surface of the layered perovskite Sr_{2}RuO_{4} under large in-plane uniaxial compression, leading to anisotropic B_{1g} strains of ϵ_{xx}-ϵ_{yy}=-0.9±0.1%. From angle-resolved photoemission, we show how this drives a sequence of Lifshitz transitions, reshaping the low-energy electronic structure and the rich spectrum of van Hove singularities that the surface layer of Sr_{2}RuO_{4} hosts. From comparison to tight-binding modeling, we find that the strain is accommodated predominantly by bond-length changes rather than modifications of octahedral tilt and rotation angles. Our study sheds new light on the nature of structural distortions at oxide surfaces, and how targeted control of these can be used to tune density of state singularities to the Fermi level, in turn paving the way to the possible realization of rich collective states at the Sr_{2}RuO_{4} surface.
Transparent conducting oxides have become ubiquitous in modern optoelectronics. However, the number of oxides that are transparent to visible light and have the metallic-like conductivity necessary for applications is limited to a handful of systems that have been known for the past 40 years. In this work, we use hybrid density functional theory and defect chemistry analysis to demonstrate that tri-rutile zinc antimonate, ZnSb2O6, is an ideal transparent conducting oxide and to identify gallium as the optimal dopant to yield high conductivity and transparency. To validate our computational predictions, we have synthesized both powder samples and single crystals of Ga-doped ZnSb2O6 which conclusively show behavior consistent with a degenerate transparent conducting oxide. This study demonstrates the possibility of a family of Sb(V)-containing oxides for transparent conducting oxide and power electronics applications.
Low-dimensional van der Waals materials have been extensively studied as a platform with which to generate quantum effects. Advancing this research, topological quantum materials with van der Waals structures are currently receiving a great deal of attention. Here, we use the concept of designing topological materials by the van der Waals stacking of quantum spin Hall insulators. Most interestingly, we find that a slight shift of inversion centre in the unit cell caused by a modification of stacking induces a transition from a trivial insulator to a higher-order topological insulator. Based on this, we present angle-resolved photoemission spectroscopy results showing that the real three-dimensional material Bi4Br4 is a higher-order topological insulator. Our demonstration that various topological states can be selected by stacking chains differently, combined with the advantages of van der Waals materials, offers a playground for engineering topologically non-trivial edge states towards future spintronics applications.
The manipulation of topological states in quantum matter is an essential pursuit of fundamental physics and next-generation quantum technology. Here we report the magnetic manipulation of Weyl fermions in the kagome spin-orbit semimetal Co_{3}Sn_{2}S_{2}, observed by high-resolution photoemission spectroscopy. We demonstrate the exchange collapse of spin-orbit-gapped ferromagnetic Weyl loops into paramagnetic Dirac loops under suppression of the magnetic order. We further observe that topological Fermi arcs disappear in the paramagnetic phase, suggesting the annihilation of exchange-split Weyl points. Our findings indicate that magnetic exchange collapse naturally drives Weyl fermion annihilation, opening new opportunities for engineering topology under correlated order parameters.
Magnetic Weyl semimetals are a newly discovered class of topological materials that may serve as a platform for exotic phenomena, such as axion insulators or the quantum anomalous Hall effect. Here, we use angle-resolved photoelectron spectroscopy and ab initio calculations to discover Weyl cones in CoS2, a ferromagnet with pyrite structure that has been long studied as a candidate for half-metallicity, which makes it an attractive material for spintronic devices. We directly observe the topological Fermi arc surface states that link the Weyl nodes, which will influence the performance of CoS2 as a spin injector by modifying its spin polarization at interfaces. In addition, we directly observe a minority-spin bulk electron pocket in the corner of the Brillouin zone, which proves that CoS2 cannot be a true half-metal.
In pnictide RbEuFe4As4, superconductivity sets in at 36 K and coexists, below 15-19 K, with the long-range magnetic ordering of Eu 4f spins. Here we report scanning tunneling experiments performed on cold-cleaved single crystals of the compound. The data revealed the coexistence of large Rb-terminated and small Eu-terminated terraces, both manifesting 1 × 2 and 2×2 reconstructions. On 2×2 surfaces, a hidden electronic order with a period â¼5 nm was discovered. A superconducting gap of â¼7 meV was seen to be strongly filled with quasiparticle states. The tunneling spectra compared with density functional theory calculations confirmed that flat electronic bands due to Eu 4f orbitals are situated â¼1.8 eV below the Fermi level and thus do not contribute directly to Cooper pair formation.
In cuprate superconductors with high critical transition temperature (T c), light hole-doping to the parent compound, which is an antiferromagnetic Mott insulator, has been predicted to lead to the formation of small Fermi pockets. These pockets, however, have not been observed. Here, we investigate the electronic structure of the five-layered Ba2Ca4Cu5O10(F,O)2, which has inner copper oxide (CuO2) planes with extremely low disorder, and find small Fermi pockets centered at (π/2, π/2) of the Brillouin zone by angle-resolved photoemission spectroscopy and quantum oscillation measurements. The d-wave superconducting gap opens along the pocket, revealing the coexistence between superconductivity and antiferromagnetic ordering in the same CuO2 sheet. These data further indicate that superconductivity can occur without contribution from the antinodal region around (π, 0), which is shared by other competing excitations.
Transition-metal dichalcogenides (TMDs) offer an ideal platform to experimentally realize Dirac fermions. However, typically these exotic quasiparticles are located far away from the Fermi level, limiting the contribution of Dirac-like carriers to the transport properties. Here we show that NiTe2 hosts both bulk Type-II Dirac points and topological surface states. The underlying mechanism is shared with other TMDs and based on the generic topological character of the Te p-orbital manifold. However, unique to NiTe2, a significant contribution of Ni d orbital states shifts the energy of the Type-II Dirac point close to the Fermi level. In addition, one of the topological surface states intersects the Fermi energy and exhibits a remarkably large spin splitting of 120 meV. Our results establish NiTe2 as an exciting candidate for next-generation spintronics devices.
It has recently been proposed that combining chirality with topological band theory results in a totally new class of fermions. Understanding how these unconventional quasiparticles propagate and interact remains largely unexplored so far. Here, we use scanning tunneling microscopy to visualize the electronic properties of the prototypical chiral topological semimetal PdGa. We reveal chiral quantum interference patterns of opposite spiraling directions for the two PdGa enantiomers, a direct manifestation of the change of sign of their Chern number. Additionally, we demonstrate that PdGa remains topologically non-trivial over a large energy range, experimentally detecting Fermi arcs in an energy window of more than 1.6 eV that is symmetrically centered around the Fermi level. These results are a consequence of the deep connection between chirality in real and reciprocal space in this class of materials, and, thereby, establish PdGa as an ideal topological chiral semimetal.
Topological semimetals feature protected nodal band degeneracies characterized by a topological invariant known as the Chern number (C). Nodal band crossings with linear dispersion are expected to have at most [Formula: see text], which sets an upper limit to the magnitude of many topological phenomena in these materials. Here, we show that the chiral crystal palladium gallium (PdGa) displays multifold band crossings, which are connected by exactly four surface Fermi arcs, thus proving that they carry the maximal Chern number magnitude of 4. By comparing two enantiomers, we observe a reversal of their Fermi-arc velocities, which demonstrates that the handedness of chiral crystals can be used to control the sign of their Chern numbers.
The possibility of triggering correlated phenomena by placing a singularity of the density of states near the Fermi energy remains an intriguing avenue toward engineering the properties of quantum materials. Twisted bilayer graphene is a key material in this regard because the superlattice produced by the rotated graphene layers introduces a van Hove singularity and flat bands near the Fermi energy that cause the emergence of numerous correlated phases, including superconductivity. Direct demonstration of electrostatic control of the superlattice bands over a wide energy range has, so far, been critically missing. This work examines the effect of electrical doping on the electronic band structure of twisted bilayer graphene using a back-gated device architecture for angle-resolved photoemission measurements with a nano-focused light spot. A twist angle of 12.2° is selected such that the superlattice Brillouin zone is sufficiently large to enable identification of van Hove singularities and flat band segments in momentum space. The doping dependence of these features is extracted over an energy range of 0.4 eV, expanding the combinations of twist angle and doping where they can be placed at the Fermi energy and thereby induce new correlated electronic phases in twisted bilayer graphene.
Quasiparticle interference (QPI) provides a wealth of information relating to the electronic structure of a material. However, it is often assumed that this information is constrained to two-dimensional electronic states. We show that this is not necessarily the case. For FeSe, a system dominated by surface defects, we show that it is actually all electronic states with negligible group velocity in the z axis that are contained within the experimental data. By using a three-dimensional tight-binding model of FeSe, fit to photoemission measurements, we directly reproduce the experimental QPI scattering dispersion, within a T-matrix formalism, by including both k_{z}=0 and k_{z}=π electronic states. This result unifies both tunnelling based and photoemission based experiments on FeSe and highlights the importance of k_{z} within surface sensitive measurements of QPI.
The charge density wave (CDW) in ZrTe_{3} is quenched in samples with a small amount of Te isoelectronically substituted by Se. Using angle-resolved photoemission spectroscopy we observe subtle changes in the electronic band dispersions and Fermi surfaces upon Se substitution. The scattering rates are substantially increased, in particular for the large three-dimensional Fermi surface sheet. The quasi-one-dimensional band is unaffected by the substitution and still shows a gap at low temperature, which starts to open from room temperature. Long-range order is, however, absent in the electronic states as in the periodic lattice distortion. The competition between superconductivity and the CDW is thus linked to the suppression of long-range order of the CDW.
We revisit the enduring problem of the 2×2×2 charge density wave (CDW) order in TiSe_{2}, utilizing photon energy-dependent angle-resolved photoemission spectroscopy to probe the full three-dimensional high- and low-temperature electronic structure. Our measurements demonstrate how a mismatch of dimensionality between the 3D conduction bands and the quasi-2D valence bands in this system leads to a hybridization that is strongly k_{z} dependent. While such a momentum-selective coupling can provide the energy gain required to form the CDW, we show how additional "passenger" states remain, which couple only weakly to the CDW and thus dominate the low-energy physics in the ordered phase of TiSe_{2}.
The ability to modulate the collective properties of correlated electron systems at their interfaces and surfaces underpins the burgeoning field of "designer" quantum materials. Here, we show how an electronic reconstruction driven by surface polarity mediates a Stoner-like magnetic instability to itinerant ferromagnetism at the Pd-terminated surface of the nonmagnetic delafossite oxide metal PdCoO2 Combining angle-resolved photoemission spectroscopy and density-functional theory calculations, we show how this leads to a rich multiband surface electronic structure. We find similar surface state dispersions in PdCrO2, suggesting surface ferromagnetism persists in this sister compound despite its bulk antiferromagnetic order.
We investigate the electronic and vibrational properties of bottom-up synthesized aligned armchair graphene nanoribbons of N = 7 carbon atoms width periodically doped by substitutional boron atoms (B-7AGNRs). Using angle-resolved photoemission spectroscopy and density functional theory calculations, we find that the dopant-derived valence and conduction band states are notably hybridized with electronic states of Au substrate and spread in energy. The interaction with the substrate leaves the bands with pure carbon character rather unperturbed. This results in an identical effective mass of ≈0.2 m0 for the next-highest valence band compared with pristine 7AGNRs. We probe the phonons of B-7AGNRs by ultrahigh-vacuum (UHV) Raman spectroscopy and reveal the existence of characteristic splitting and red shifts in Raman modes due to the presence of substitutional boron atoms. Comparing the Raman spectra for three visible lasers (red, green, and blue), we find that interaction with gold suppresses the Raman signal from B-7AGNRs and the energy of the green laser (2.33 eV) is closer to the resonant E22 transition. The hybridized electronic structure of the B-7AGNR-Au interface is expected to improve electrical characteristics of contacts between graphene nanoribbon and Au. The Raman fingerprint allows the easy identification of B-7AGNRs, which is particularly useful for device fabrication.
How the interacting electronic states and phases of layered transition-metal dichalcogenides evolve when thinned to the single-layer limit is a key open question in the study of two-dimensional materials. Here, we use angle-resolved photoemission to investigate the electronic structure of monolayer VSe2 grown on bilayer graphene/SiC. While the global electronic structure is similar to that of bulk VSe2, we show that, for the monolayer, pronounced energy gaps develop over the entire Fermi surface with decreasing temperature below Tc = 140 ± 5 K, concomitant with the emergence of charge-order superstructures evident in low-energy electron diffraction. These observations point to a charge-density wave instability in the monolayer that is strongly enhanced over that of the bulk. Moreover, our measurements of both the electronic structure and of X-ray magnetic circular dichroism reveal no signatures of a ferromagnetic ordering, in contrast to the results of a recent experimental study as well as expectations from density functional theory. Our study thus points to a delicate balance that can be realized between competing interacting states and phases in monolayer transition-metal dichalcogenides.
Two-dimensional (2D) crystals have emerged as a class of materials with tunable carrier density1. Carrier doping to 2D semiconductors can be used to modulate many-body interactions2 and to explore novel composite particles. The Holstein polaron is a small composite particle of an electron that carries a cloud of self-induced lattice deformation (or phonons)3-5, which has been proposed to play a key role in high-temperature superconductivity6 and carrier mobility in devices7. Here we report the discovery of Holstein polarons in a surface-doped layered semiconductor, MoS2, in which a puzzling 2D superconducting dome with the critical temperature of 12 K was found recently8-11. Using a high-resolution band mapping of charge carriers, we found strong band renormalizations collectively identified as a hitherto unobserved spectral function of Holstein polarons12-18. The short-range nature of electron-phonon (e-ph) coupling in MoS2 can be explained by its valley degeneracy, which enables strong intervalley coupling mediated by acoustic phonons. The coupling strength is found to increase gradually along the superconducting dome up to the intermediate regime, which suggests a bipolaronic pairing in the 2D superconductivity.
