Anomalous intense coherent secondary photoemission from a perovskite oxide.

Photocathodes-materials that convert photons into electrons through a phenomenon known as the photoelectric effect-are important for many modern technologies that rely on light detection or electron-beam generation1-3. However, current photocathodes are based on conventional metals and semiconductors that were mostly discovered six decades ago with sound theoretical underpinnings4,5. Progress in this field has been limited to refinements in photocathode performance based on sophisticated materials engineering1,6. Here we report unusual photoemission properties of the reconstructed surface of single crystals of the perovskite oxide SrTiO3(100), which were prepared by simple vacuum annealing. These properties are different from the existing theoretical descriptions4,7-10. In contrast to other photocathodes with a positive electron affinity, our SrTiO3 surface produces, at room temperature, discrete secondary photoemission spectra, which are characteristic of efficient photocathode materials with a negative electron affinity11,12. At low temperatures, the photoemission peak intensity is enhanced substantially and the electron beam obtained from non-threshold excitations shows longitudinal and transverse coherence that differs from previous results by at least an order of magnitude6,13,14. The observed emergence of coherence in secondary photoemission points to the development of a previously undescribed underlying process in addition to those of the current theoretical photoemission framework. SrTiO3 is an example of a fundamentally new class of photocathode quantum materials that could be used for applications that require intense coherent electron beams, without the need for monochromatic excitations.

Tomographic reconstruction of oxygen orbitals in lithium-rich battery materials.

The electrification of heavy-duty transport and aviation will require new strategies to increase the energy density of electrode materials1,2. The use of anionic redox represents one possible approach to meeting this ambitious target. However, questions remain regarding the validity of the O2-/O- oxygen redox paradigm, and alternative explanations for the origin of the anionic capacity have been proposed3, because the electronic orbitals associated with redox reactions cannot be measured by standard experiments. Here, using high-energy X-ray Compton measurements together with first-principles modelling, we show how the electronic orbital that lies at the heart of the reversible and stable anionic redox activity can be imaged and visualized, and its character and symmetry determined. We find that differential changes in the Compton profile with lithium-ion concentration are sensitive to the phase of the electronic wave function, and carry signatures of electrostatic and covalent bonding effects4. Our study not only provides a picture of the workings of a lithium-rich battery at the atomic scale, but also suggests pathways to improving existing battery materials and designing new ones.

Layer Hall effect in a 2D topological axion antiferromagnet.

Whereas ferromagnets have been known and used for millennia, antiferromagnets were only discovered in the 1930s1. At large scale, because of the absence of global magnetization, antiferromagnets may seem to behave like any non-magnetic material. At the microscopic level, however, the opposite alignment of spins forms a rich internal structure. In topological antiferromagnets, this internal structure leads to the possibility that the property known as the Berry phase can acquire distinct spatial textures2,3. Here we study this possibility in an antiferromagnetic axion insulator-even-layered, two-dimensional MnBi2Te4-in which spatial degrees of freedom correspond to different layers. We observe a type of Hall effect-the layer Hall effect-in which electrons from the top and bottom layers spontaneously deflect in opposite directions. Specifically, under zero electric field, even-layered MnBi2Te4 shows no anomalous Hall effect. However, applying an electric field leads to the emergence of a large, layer-polarized anomalous Hall effect of about 0.5e2/h (where e is the electron charge and h is Planck's constant). This layer Hall effect uncovers an unusual layer-locked Berry curvature, which serves to characterize the axion insulator state. Moreover, we find that the layer-locked Berry curvature can be manipulated by the axion field formed from the dot product of the electric and magnetic field vectors. Our results offer new pathways to detect and manipulate the internal spatial structure of fully compensated topological antiferromagnets4-9. The layer-locked Berry curvature represents a first step towards spatial engineering of the Berry phase through effects such as layer-specific moiré potential.

Axion optical induction of antiferromagnetic order.

Using circularly polarized light to control quantum matter is a highly intriguing topic in physics, chemistry and biology. Previous studies have demonstrated helicity-dependent optical control of chirality and magnetization, with important implications in asymmetric synthesis in chemistry; homochirality in biomolecules; and ferromagnetic spintronics. We report the surprising observation of helicity-dependent optical control of fully compensated antiferromagnetic order in two-dimensional even-layered MnBi2Te4, a topological axion insulator with neither chirality nor magnetization. To understand this control, we study an antiferromagnetic circular dichroism, which appears only in reflection but is absent in transmission. We show that the optical control and circular dichroism both arise from the optical axion electrodynamics. Our axion induction provides the possibility to optically control a family of [Formula: see text]-symmetric antiferromagnets ([Formula: see text], inversion; [Formula: see text], time-reversal) such as Cr2O3, even-layered CrI3 and possibly the pseudo-gap state in cuprates. In MnBi2Te4, this further opens the door for optical writing of a dissipationless circuit formed by topological edge states.

Emergence of Competing Stripe Phases in Undoped Infinite-Layer Nickelates.

Recent discovery of superconductivity in infinite-layer nickelates has ignited renewed theoretical and experimental interest in the role of electronic correlations in their properties. Here, using first-principles simulations, we show that the parent compound of the nickelate family, LaNiO_{2}, hosts competing low-energy stripe phases, similar to doped cuprates. The stripe states are shown to be driven by multiorbital electronic mechanisms and Peierls distortions. Our study indicates that both strong correlations and electron-phonon coupling effects play a key role in the physics of infinite-layer nickelates, and sheds light on the microscopic origin of electronic inhomogeneity and the lack of long-range order in the nickelates.

Comparing first-principles density functionals plus corrections for the lattice dynamics of YBa2Cu3O6.

The enigmatic mechanism underlying unconventional high-temperature superconductivity, especially the role of lattice dynamics, has remained a subject of debate. Theoretical insights have long been hindered due to the lack of an accurate first-principles description of the lattice dynamics of cuprates. Recently, using the r2SCAN meta-generalized gradient approximation (meta-GGA) functional, we have been able to achieve accurate phonon spectra of an insulating cuprate YBa2Cu3O6 and discover significant magnetoelastic coupling in experimentally interesting Cu-O bond stretching optical modes [Ning et al., Phys. Rev. B 107, 045126 (2023)]. We extend this work by comparing Perdew-Burke-Ernzerhof and r2SCAN performances with corrections from the on-site Hubbard U and the D4 van der Waals (vdW) methods, aiming at further understanding on both the materials science side and the density functional side. We demonstrate the importance of vdW and self-interaction corrections for accurate first-principles YBa2Cu3O6 lattice dynamics. Since r2SCAN by itself partially accounts for these effects, the good performance of r2SCAN is now more fully explained. In addition, the performances of the Tao-Mo series of meta-GGAs, which are constructed in a different way from the strongly constrained and appropriately normed (SCAN) meta-GGA and its revised version r2SCAN, are also compared and discussed.

Discovery of a Magnetic Dirac System with a Large Intrinsic Nonlinear Hall Effect.

Magnetic materials exhibiting topological Dirac fermions are attracting significant attention for their promising technological potential in spintronics. In these systems, the combined effect of the spin-orbit coupling and magnetic order enables the realization of novel topological phases with exotic transport properties, including the anomalous Hall effect and magneto-chiral phenomena. Herein, we report experimental signature of topological Dirac antiferromagnetism in TaCoTe2 via angle-resolved photoelectron spectroscopy and first-principles density functional theory calculations. In particular, we find the existence of spin-orbit coupling-induced gaps at the Fermi level, consistent with the manifestation of a large intrinsic nonlinear Hall conductivity. Remarkably, we find that the latter is extremely sensitive to the orientation of the Néel vector, suggesting TaCoTe2 as a suitable candidate for the realization of non-volatile spintronic devices with an unprecedented level of intrinsic tunability.

Coexistence of Bulk-Nodal and Surface-Nodeless Cooper Pairings in a Superconducting Dirac Semimetal.

The interplay of nontrivial topology and superconductivity in condensed matter physics gives rise to exotic phenomena. However, materials are extremely rare where it is possible to explore the full details of the superconducting pairing. Here, we investigate the momentum dependence of the superconducting gap distribution in a novel Dirac material PdTe. Using high resolution, low temperature photoemission spectroscopy, we establish it as a spin-orbit coupled Dirac semimetal with the topological Fermi arc crossing the Fermi level on the (010) surface. This spin-textured surface state exhibits a fully gapped superconducting Cooper pairing structure below T_{c}∼4.5 K. Moreover, we find a node in the bulk near the Brillouin zone boundary, away from the topological Fermi arc. These observations not only demonstrate the band resolved electronic correlation between topological Fermi arc states and the way it induces Cooper pairing in PdTe, but also provide a rare case where surface and bulk states host a coexistence of nodeless and nodal gap structures enforced by spin-orbit coupling.

Competing stripe and magnetic phases in the cuprates from first principles.

Realistic description of competing phases in complex quantum materials has proven extremely challenging. For example, much of the existing density-functional-theory-based first-principles framework fails in the cuprate superconductors. Various many-body approaches involve generic model Hamiltonians and do not account for the interplay between the spin, charge, and lattice degrees of freedom. Here, by deploying the recently constructed strongly constrained and appropriately normed (SCAN) density functional, we show how the landscape of competing stripe and magnetic phases can be addressed on a first-principles basis both in the parent insulator YBa2Cu3O6 and the near-optimally doped YBa2Cu3O7 as archetype cuprate compounds. In YBa2Cu3O7, we find many stripe phases that are nearly degenerate with the ground state and may give rise to the pseudogap state from which the high-temperature superconducting state emerges. We invoke no free parameters such as the Hubbard U, which has been the basis of much of the existing cuprate literature. Lattice degrees of freedom are found to be crucially important in stabilizing the various phases.

Re-examining the giant magnetization density in α''-Fe16N2 with the SCAN+U method.

We present an in-depth discussion of the magnetic ground state of α''-Fe16N2 within the framework of the density functional theory (DFT). The exchange-correlation effects are treated using a variety of schemes, including the local-spin-density approximation, the generalized-gradient approximation, and the Strongly-Constrained-and-Appropriately-Normed (SCAN) scheme. We also delineate effects of adding an on-site interaction parameter U on the Fe sites. Among all the schemes considered, only SCAN+U is found to capture the surprisingly large magnetization density in α''-Fe16N2 that has been observed experimentally. Our study shows how the combination of SCAN and self-interaction corrections applied on different Fe sites through the parameter U can reproduce both the correct equilibrium volume and the giant magnetization density of α''-Fe16N2.

Topology on a new facet of bismuth.

Bismuth-based materials have been instrumental in the development of topological physics, even though bulk bismuth itself has been long thought to be topologically trivial. A recent study has, however, shown that bismuth is in fact a higher-order topological insulator featuring one-dimensional (1D) topological hinge states protected by threefold rotational and inversion symmetries. In this paper, we uncover another hidden facet of the band topology of bismuth by showing that bismuth is also a first-order topological crystalline insulator protected by a twofold rotational symmetry. As a result, its [Formula: see text] surface exhibits a pair of gapless Dirac surface states. Remarkably, these surface Dirac cones are "unpinned" in the sense that they are not restricted to locate at specific k points in the [Formula: see text] surface Brillouin zone. These unpinned 2D Dirac surface states could be probed directly via various spectroscopic techniques. Our analysis also reveals the presence of a distinct, previously uncharacterized set of 1D topological hinge states protected by the twofold rotational symmetry. Our study thus provides a comprehensive understanding of the topological band structure of bismuth.

New type of Weyl semimetal with quadratic double Weyl fermions.

Weyl semimetals have attracted worldwide attention due to their wide range of exotic properties predicted in theories. The experimental realization had remained elusive for a long time despite much effort. Very recently, the first Weyl semimetal has been discovered in an inversion-breaking, stoichiometric solid TaAs. So far, the TaAs class remains the only Weyl semimetal available in real materials. To facilitate the transition of Weyl semimetals from the realm of purely theoretical interest to the realm of experimental studies and device applications, it is of crucial importance to identify other robust candidates that are experimentally feasible to be realized. In this paper, we propose such a Weyl semimetal candidate in an inversion-breaking, stoichiometric compound strontium silicide, SrSi2, with many new and novel properties that are distinct from TaAs. We show that SrSi2 is a Weyl semimetal even without spin-orbit coupling and that, after the inclusion of spin-orbit coupling, two Weyl fermions stick together forming an exotic double Weyl fermion with quadratic dispersions and a higher chiral charge of ±2. Moreover, we find that the Weyl nodes with opposite charges are located at different energies due to the absence of mirror symmetry in SrSi2, paving the way for the realization of the chiral magnetic effect. Our systematic results not only identify a much-needed robust Weyl semimetal candidate but also open the door to new topological Weyl physics that is not possible in TaAs.

Direct evidence of interaction-induced Dirac cones in a monolayer silicene/Ag(111) system.

Silicene, analogous to graphene, is a one-atom-thick 2D crystal of silicon, which is expected to share many of the remarkable properties of graphene. The buckled honeycomb structure of silicene, along with enhanced spin-orbit coupling, endows silicene with considerable advantages over graphene in that the spin-split states in silicene are tunable with external fields. Although the low-energy Dirac cone states lie at the heart of all novel quantum phenomena in a pristine sheet of silicene, a hotly debated question is whether these key states can survive when silicene is grown or supported on a substrate. Here we report our direct observation of Dirac cones in monolayer silicene grown on a Ag(111) substrate. By performing angle-resolved photoemission measurements on silicene(3 × 3)/Ag(111), we reveal the presence of six pairs of Dirac cones located on the edges of the first Brillouin zone of Ag(111), which is in sharp contrast to the expected six Dirac cones centered at the K points of the primary silicene(1 × 1) Brillouin zone. Our analysis shows clearly that the unusual Dirac cone structure we have observed is not tied to pristine silicene alone but originates from the combined effects of silicene(3 × 3) and the Ag(111) substrate. Our study thus identifies the case of a unique type of Dirac cone generated through the interaction of two different constituents. The observation of Dirac cones in silicene/Ag(111) opens a unique materials platform for investigating unusual quantum phenomena and for applications based on 2D silicon systems.

Topological Hourglass Dirac Semimetal in the Nonpolar Phase of Ag_{2}BiO_{3}.

Materials with tunable charge and lattice degrees of freedom provide excellent platforms for investigating multiple phases that can be controlled via external stimuli. We show how the charge-ordered ferroelectric oxide Ag_{2}BiO_{3}, which has been realized experimentally, presents a unique exemplar of a metal-insulator transition under an external electric field. Our first-principles calculations, combined with a symmetry analysis, reveal the presence of a nearly ideal hourglass-Dirac-semimetal state in the nonpolar structure of Ag_{2}BiO_{3}. The low-energy band structure consists of two hourglasslike nodal lines located on two mutually orthogonal glide-mirror planes in the absence of spin-orbit coupling (SOC) effects. These lines cross at a common point and form an interlinked chainlike structure, which extends beyond the first Brillouin zone. Inclusion of the SOC opens a small gap in the nodal lines and results in two symmetry-enforced hourglasslike Dirac points on the C[over ˜]_{2y} screw rotation axis. Our results indicate that Ag_{2}BiO_{3} will provide an ideal platform for exploring the ferroelectric-semiconductor to Dirac-semimetal transition by the application of an external electric field.

Nature of the Positron State in CdSe Quantum Dots.

Previous studies have shown that positron-annihilation spectroscopy is a highly sensitive probe of the electronic structure and surface composition of ligand-capped semiconductor quantum dots (QDs) embedded in thin films. The nature of the associated positron state, however, whether the positron is confined inside the QDs or localized at their surfaces, has so far remained unresolved. Our positron-annihilation lifetime spectroscopy studies of CdSe QDs reveal the presence of a strong lifetime component in the narrow range of 358-371 ps, indicating abundant trapping and annihilation of positrons at the surfaces of the QDs. Furthermore, our ab initio calculations of the positron wave function and lifetime employing a recent formulation of the weighted density approximation demonstrate the presence of a positron surface state and predict positron lifetimes close to experimental values. Our study thus resolves the long-standing question regarding the nature of the positron state in semiconductor QDs and opens the way to extract quantitative information on surface composition and ligand-surface interactions of colloidal semiconductor QDs through highly sensitive positron-annihilation techniques.

Topological Hopf and Chain Link Semimetal States and Their Application to Co_{2}MnGa.

Topological semimetals can be classified by the connectivity and dimensionality of the band crossings in momentum space. The band crossings of a Dirac, Weyl, or an unconventional fermion semimetal are zero-dimensional (0D) points, whereas the band crossings of a nodal-line semimetal are one-dimensional (1D) closed loops. Here we propose that the presence of perpendicular crystalline mirror planes can protect three-dimensional (3D) band crossings characterized by nontrivial links such as a Hopf link or a coupled chain, giving rise to a variety of new types of topological semimetals. We show that the nontrivial winding number protects topological surface states distinct from those in previously known topological semimetals with a vanishing spin-orbit interaction. We also show that these nontrivial links can be engineered by tuning the mirror eigenvalues associated with the perpendicular mirror planes. Using first-principles band structure calculations, we predict the ferromagnetic full Heusler compound Co_{2}MnGa as a candidate. Both Hopf link and chainlike bulk band crossings and unconventional topological surface states are identified.

Quasiparticle Interference on Cubic Perovskite Oxide Surfaces.

We report the observation of coherent surface states on cubic perovskite oxide SrVO_{3}(001) thin films through spectroscopic-imaging scanning tunneling microscopy. A direct link between the observed quasiparticle interference patterns and the formation of a d_{xy}-derived surface state is supported by first-principles calculations. We show that the apical oxygens on the topmost VO_{2} plane play a critical role in controlling the coherent surface state via modulating orbital state.

Unconventional Chiral Fermions and Large Topological Fermi Arcs in RhSi.

The theoretical proposal of chiral fermions in topological semimetals has led to a significant effort towards their experimental realization. In particular, the Fermi surfaces of chiral semimetals carry quantized Chern numbers, making them an attractive platform for the observation of exotic transport and optical phenomena. While the simplest example of a chiral fermion in condensed matter is a conventional |C|=1 Weyl fermion, recent theoretical works have proposed a number of unconventional chiral fermions beyond the standard model which are protected by unique combinations of topology and crystalline symmetries. However, materials candidates for experimentally probing the transport and response signatures of these unconventional fermions have thus far remained elusive. In this Letter, we propose the RhSi family in space group No. 198 as the ideal platform for the experimental examination of unconventional chiral fermions. We find that RhSi is a filling-enforced semimetal that features near its Fermi surface a chiral double sixfold-degenerate spin-1 Weyl node at R and a previously uncharacterized fourfold-degenerate chiral fermion at Γ. Each unconventional fermion displays Chern number ±4 at the Fermi level. We also show that RhSi displays the largest possible momentum separation of compensative chiral fermions, the largest proposed topologically nontrivial energy window, and the longest possible Fermi arcs on its surface. We conclude by proposing signatures of an exotic bulk photogalvanic response in RhSi.

Dirac mass generation from crystal symmetry breaking on the surfaces of topological crystalline insulators.

The tunability of topological surface states and controllable opening of the Dirac gap are of fundamental and practical interest in the field of topological materials. In the newly discovered topological crystalline insulators (TCIs), theory predicts that the Dirac node is protected by a crystalline symmetry and that the surface state electrons can acquire a mass if this symmetry is broken. Recent studies have detected signatures of a spontaneously generated Dirac gap in TCIs; however, the mechanism of mass formation remains elusive. In this work, we present scanning tunnelling microscopy (STM) measurements of the TCI Pb1-xSnxSe for a wide range of alloy compositions spanning the topological and non-topological regimes. The STM topographies reveal a symmetry-breaking distortion on the surface, which imparts mass to the otherwise massless Dirac electrons-a mechanism analogous to the long sought-after Higgs mechanism in particle physics. Interestingly, the measured Dirac gap decreases on approaching the trivial phase, whereas the magnitude of the distortion remains nearly constant. Our data and calculations reveal that the penetration depth of Dirac surface states controls the magnitude of the Dirac mass. At the limit of the critical composition, the penetration depth is predicted to go to infinity, resulting in zero mass, consistent with our measurements. Finally, we discover the existence of surface states in the non-topological regime, which have the characteristics of gapped, double-branched Dirac fermions and could be exploited in realizing superconductivity in these materials.

Atomic-Scale Visualization of Quasiparticle Interference on a Type-II Weyl Semimetal Surface.

We combine quasiparticle interference simulation (theory) and atomic resolution scanning tunneling spectromicroscopy (experiment) to visualize the interference patterns on a type-II Weyl semimetal Mo_{x}W_{1-x}Te_{2} for the first time. Our simulation based on first-principles band topology theoretically reveals the surface electron scattering behavior. We identify the topological Fermi arc states and reveal the scattering properties of the surface states in Mo_{0.66}W_{0.34}Te_{2}. In addition, our result reveals an experimental signature of the topology via the interconnectivity of bulk and surface states, which is essential for understanding the unusual nature of this material.