Weyl spin-momentum locking in a chiral topological semimetal.

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.

Direct observation of altermagnetic band splitting in CrSb thin films.

Altermagnetism represents an emergent collinear magnetic phase with compensated order and an unconventional alternating even-parity wave spin order in the non-relativistic band structure. We investigate directly this unconventional band splitting near the Fermi energy through spin-integrated soft X-ray angular resolved photoemission spectroscopy. The experimentally obtained angle-dependent photoemission intensity, acquired from epitaxial thin films of the predicted altermagnet CrSb, demonstrates robust agreement with the corresponding band structure calculations. In particular, we observe the distinctive splitting of an electronic band on a low-symmetry path in the Brilliouin zone that connects two points featuring symmetry-induced degeneracy. The measured large magnitude of the spin splitting of approximately 0.6 eV and the position of the band just below the Fermi energy underscores the significance of altermagnets for spintronics based on robust broken time reversal symmetry responses arising from exchange energy scales, akin to ferromagnets, while remaining insensitive to external magnetic fields and possessing THz dynamics, akin to antiferromagnets.

Tunable 2D Electron- and 2D Hole States Observed at Fe/SrTiO3 Interfaces.

Oxide electronics provide the key concepts and materials for enhancing silicon-based semiconductor technologies with novel functionalities. However, a basic but key property of semiconductor devices still needs to be unveiled in its oxidic counterparts: the ability to set or even switch between two types of carriers-either negatively (n) charged electrons or positively (p) charged holes. Here, direct evidence for individually emerging n- or p-type 2D band dispersions in STO-based heterostructures is provided using resonant photoelectron spectroscopy. The key to tuning the carrier character is the oxidation state of an adjacent Fe-based interface layer: For Fe and FeO, hole bands emerge in the empty bandgap region of STO due to hybridization of Ti- and Fe- derived states across the interface, while for Fe3O4 overlayers, an 2D electron system is formed. Unexpected oxygen vacancy characteristics arise for the hole-type interfaces, which as of yet had been exclusively assigned to the emergence of 2DESs. In general, this finding opens up the possibility to straightforwardly switch the type of conductivity at STO interfaces by the oxidation state of a redox overlayer. This will extend the spectrum of phenomena in oxide electronics, including the realization of combined n/p-type all-oxide transistors or logic gates.

Nematic Spin Correlations Pervading the Phase Diagram of FeSe_{1-x}S_{x}.

We use resonant inelastic x-ray scattering (RIXS) at the Fe-L_{3} edge to study the spin excitations of uniaxial-strained and unstrained FeSe_{1-x}S_{x} (0≤x≤0.21) samples. The measurements on unstrained samples reveal dispersive spin excitations in all doping levels, which show only minor doping dependence in energy dispersion, lifetime, and intensity, indicating that high-energy spin excitations are only marginally affected by sulfur doping. RIXS measurements on uniaxial-strained samples reveal that the high-energy spin-excitation anisotropy observed previously in FeSe is also present in the doping range 0200 K in x=0.18 and reaches a maximum around the nematic quantum critical doping (x_{c}≈0.17). Since the spin-excitation anisotropy directly reflects the existence of nematic spin correlations, our results indicate that high-energy nematic spin correlations pervade the regime of nematicity in the phase diagram and are enhanced by the nematic quantum criticality. These results emphasize the essential role of spin fluctuations in driving electronic nematicity and highlight the capability of uniaxial strain in tuning spin excitations in quantum materials hosting strong magnetoelastic coupling and electronic nematicity.

Momentum-Space Imaging of Ultra-Thin Electron Liquids in δ-Doped Silicon.

Two-dimensional dopant layers (δ-layers) in semiconductors provide the high-mobility electron liquids (2DELs) needed for nanoscale quantum-electronic devices. Key parameters such as carrier densities, effective masses, and confinement thicknesses for 2DELs have traditionally been extracted from quantum magnetotransport. In principle, the parameters are immediately readable from the one-electron spectral function that can be measured by angle-resolved photoemission spectroscopy (ARPES). Here, buried 2DEL δ-layers in silicon are measured with soft X-ray (SX) ARPES to obtain detailed information about their filled conduction bands and extract device-relevant properties. This study takes advantage of the larger probing depth and photon energy range of SX-ARPES relative to vacuum ultraviolet (VUV) ARPES to accurately measure the δ-layer electronic confinement. The measurements are made on ambient-exposed samples and yield extremely thin (< 1 nm) and dense (≈1014  cm-2 ) 2DELs. Critically, this method is used to show that δ-layers of arsenic exhibit better electronic confinement than δ-layers of phosphorus fabricated under identical conditions.

Interplay between Magnetism and Topology: Large Topological Hall Effect in an Antiferromagnetic Topological Insulator, EuCuAs.

Magnetic interactions in combination with nontrivial band structures can give rise to several exotic physical properties such as a large anomalous Hall effect, the anomalous Nernst effect, and the topological Hall effect (THE). Antiferromagnetic (AFM) materials exhibit the THE due to the presence of nontrivial spin structures. EuCuAs crystallizes in a hexagonal structure with an AFM ground state (Néel temperature ∼ 16 K). In this work, we observe a large topological Hall resistivity of ∼7.4 µΩ-cm at 13 K which is significantly higher than the giant topological Hall effect of Gd2PdSi3 (∼3 µΩ-cm). Neutron diffraction experiments reveal that the spins form a transverse conical structure during the metamagnetic transition, resulting in the large THE. In addition, by controlling the magnetic ordering structure of EuCuAs with an external magnetic field, several fascinating topological states such as Dirac and Weyl semimetals have been revealed. These results suggest the possibility of spintronic devices based on antiferromagnets with tailored noncoplanar spin configurations.

First-Principles Assessment of CdTe as a Tunnel Barrier at the α-Sn/InSb Interface.

Majorana zero modes, with prospective applications in topological quantum computing, are expected to arise in superconductor/semiconductor interfaces, such as ß-Sn and InSb. However, proximity to the superconductor may also adversely affect the semiconductor's local properties. A tunnel barrier inserted at the interface could resolve this issue. We assess the wide band gap semiconductor, CdTe, as a candidate material to mediate the coupling at the lattice-matched interface between α-Sn and InSb. To this end, we use density functional theory (DFT) with Hubbard U corrections, whose values are machine-learned via Bayesian optimization (BO) [ npj Computational Materials 2020, 6, 180]. The results of DFT+U(BO) are validated against angle resolved photoemission spectroscopy (ARPES) experiments for α-Sn and CdTe. For CdTe, the z-unfolding method [ Advanced Quantum Technologies 2022, 5, 2100033] is used to resolve the contributions of different kz values to the ARPES. We then study the band offsets and the penetration depth of metal-induced gap states (MIGS) in bilayer interfaces of InSb/α-Sn, InSb/CdTe, and CdTe/α-Sn, as well as in trilayer interfaces of InSb/CdTe/α-Sn with increasing thickness of CdTe. We find that 16 atomic layers (3.5 nm) of CdTe can serve as a tunnel barrier, effectively shielding the InSb from MIGS from the α-Sn. This may guide the choice of dimensions of the CdTe barrier to mediate the coupling in semiconductor-superconductor devices in future Majorana zero modes experiments.

Visualizing Higher-Fold Topology in Chiral Crystals.

Novel topological phases of matter are fruitful platforms for the discovery of unconventional electromagnetic phenomena. Higher-fold topology is one example, where the low-energy description goes beyond standard model analogs. Despite intensive experimental studies, conclusive evidence remains elusive for the multigap topological nature of higher-fold chiral fermions. In this Letter, we leverage a combination of fine-tuned chemical engineering and photoemission spectroscopy with photon energy contrast to discover the higher-fold topology of a chiral crystal. We identify all bulk branches of a higher-fold chiral fermion for the first time, critically important for allowing us to explore unique Fermi arc surface states in multiple interband gaps, which exhibit an emergent ladder structure. Through designer chemical gating of the samples in combination with our measurements, we uncover an unprecedented multigap bulk boundary correspondence. Our demonstration of multigap electronic topology will propel future research on unconventional topological responses.

Anomalous Hall Conductivity and Nernst Effect of the Ideal Weyl Semimetallic Ferromagnet EuCd2 As2.

Weyl semimetal is a unique topological phase with topologically protected band crossings in the bulk and robust surface states called Fermi arcs. Weyl nodes always appear in pairs with opposite chiralities, and they need to have either time-reversal or inversion symmetry broken. When the time-reversal symmetry is broken the minimum number of Weyl points (WPs) is two. If these WPs are located at the Fermi level, they form an ideal Weyl semimetal (WSM). In this study, intrinsic ferromagnetic (FM) EuCd2 As2 are grown, predicted to be an ideal WSM and studied its electronic structure by angle-resolved photoemission spectroscopy, and scanning tunneling microscopy which agrees closely with the first principles calculations. Moreover, anomalous Hall conductivity and Nernst effect are observed, resulting from the non-zero Berry curvature, and the topological Hall effect arising from changes in the band structure caused by spin canting produced by magnetic fields. These findings can help realize several exotic quantum phenomena in inorganic topological materials that are otherwise difficult to assess because of the presence of multiple pairs of Weyl nodes.

Experimental Band Structure of Pb(Zr,Ti)O3 : Mechanism of Ferroelectric Stabilization.

Pb(Zr,Ti)O3 (PZT) is the most common ferroelectric (FE) material widely used in solid-state technology. Despite intense studies of PZT over decades, its intrinsic band structure, electron energy depending on 3D momentum k, is still unknown. Here, Pb(Zr0.2 Ti0.8 )O3 using soft-X-ray angle-resolved photoelectron spectroscopy (ARPES) is explored. The enhanced photoelectron escape depth in this photon energy range allows sharp intrinsic definition of the out-of-plane momentum k and thereby of the full 3D band structure. Furthermore, the problem of sample charging due to the inherently insulating nature of PZT is solved by using thin-film PZT samples, where a thickness-induced self-doping results in their heavy doping. For the first time, the soft-X-ray ARPES experiments deliver the intrinsic 3D band structure of PZT as well as the FE-polarization dependent electrostatic potential profile across the PZT film deposited on SrTiO3 and Lax SrMn1- x O3 substrates. The negative charges near the surface, required to stabilize the FE state pointing away from the sample (P+), are identified as oxygen vacancies creating localized in-gap states below the Fermi energy. For the opposite polarization state (P-), the positive charges near the surface are identified as cation vacancies resulting from non-ideal stoichiometry of the PZT film as deduced from quantitative XPS measurements.

Visualization of Tunable Weyl Line in A-A Stacking Kagome Magnets.

Kagome magnets provide a fascinating platform for a plethora of topological quantum phenomena, in which the delicate interplay between frustrated crystal structure, magnetization, and spin-orbit coupling (SOC) can engender highly tunable topological states. Here, utilizing angle-resolved photoemission spectroscopy, the Weyl lines are directly visualized with strong out-of-plane dispersion in the A-A stacked kagome magnet GdMn6 Sn6 . Remarkably, the Weyl lines exhibit a strong magnetization-direction-tunable SOC gap and binding energy tunability after substituting Gd with Tb and Li, respectively. These results not only illustrate the magnetization direction and valence counting as efficient tuning knobs for realizing and controlling distinct 3D topological phases, but also demonstrate AMn6 Sn6 (A = rare earth, or Li, Mg, or Ca) as a versatile material family for exploring diverse emergent topological quantum responses.

Charge fluctuations in the intermediate-valence ground state of SmCoIn5.

The microscopic mechanism of heavy band formation, relevant for unconventional superconductivity in CeCoIn5 and other Ce-based heavy fermion materials, depends strongly on the efficiency with which f electrons are delocalized from the rare earth sites and participate in a Kondo lattice. Replacing Ce3+ (4f1, J = 5/2) with Sm3+ (4f5, J = 5/2), we show that a combination of the crystal electric field and on-site Coulomb repulsion causes SmCoIn5 to exhibit a Γ7 ground state similar to CeCoIn5 with multiple f electrons. We show that with this single-ion ground state, SmCoIn5 exhibits a temperature-induced valence crossover consistent with a Kondo scenario, leading to increased delocalization of f holes below a temperature scale set by the crystal field, Tv ≈ 60 K. Our result provides evidence that in the case of many f electrons, the crystal field remains the dominant tuning knob in controlling the efficiency of delocalization near a heavy fermion quantum critical point, and additionally clarifies that charge fluctuations play a general role in the ground state of "115" materials.

Momentum-resolved spin-conserving two-triplon bound state and continuum in a cuprate ladder.

Studying multi-particle elementary excitations has provided unique access to understand collective many-body phenomena in correlated electronic materials, paving the way towards constructing microscopic models. In this work, we perform O K-edge resonant inelastic X-ray scattering (RIXS) on the quasi-one-dimensional cuprate Sr14Cu24O41 with weakly-doped spin ladders. The RIXS signal is dominated by a dispersing sharp mode ~ 270 meV on top of a damped incoherent component ~ 400-500 meV. Comparing with model calculations using the perturbative continuous unitary transformations method, the two components resemble the spin-conserving ΔS = 0 two-triplon bound state and continuum excitations in the spin ladders. Such multi-spin response with long-lived ΔS = 0 excitons is central to several exotic magnetic properties featuring Majorana fermions, yet remains unexplored given the generally weak cross-section with other experimental techniques. By investigating a simple spin-ladder model system, our study provides valuable insight into low-dimensional quantum magnetism.

Observation of a linked-loop quantum state in a topological magnet.

Quantum phases can be classified by topological invariants, which take on discrete values capturing global information about the quantum state1-13. Over the past decades, these invariants have come to play a central role in describing matter, providing the foundation for understanding superfluids5, magnets6,7, the quantum Hall effect3,8, topological insulators9,10, Weyl semimetals11-13 and other phenomena. Here we report an unusual linking-number (knot theory) invariant associated with loops of electronic band crossings in a mirror-symmetric ferromagnet14-20. Using state-of-the-art spectroscopic methods, we directly observe three intertwined degeneracy loops in the material's three-torus, T3, bulk Brillouin zone. We find that each loop links each other loop twice. Through systematic spectroscopic investigation of this linked-loop quantum state, we explicitly draw its link diagram and conclude, in analogy with knot theory, that it exhibits the linking number (2, 2, 2), providing a direct determination of the invariant structure from the experimental data. We further predict and observe, on the surface of our samples, Seifert boundary states protected by the bulk linked loops, suggestive of a remarkable Seifert bulk-boundary correspondence. Our observation of a quantum loop link motivates the application of knot theory to the exploration of magnetic and superconducting quantum matter.

Electron-momentum dependence of electron-phonon coupling underlies dramatic phonon renormalization in YNi2B2C.

Electron-phonon coupling, i.e., the scattering of lattice vibrations by electrons and vice versa, is ubiquitous in solids and can lead to emergent ground states such as superconductivity and charge-density wave order. A broad spectral phonon line shape is often interpreted as a marker of strong electron-phonon coupling associated with Fermi surface nesting, i.e., parallel sections of the Fermi surface connected by the phonon momentum. Alternatively broad phonons are known to arise from strong atomic lattice anharmonicity. Here, we show that strong phonon broadening can occur in the absence of both Fermi surface nesting and lattice anharmonicity, if electron-phonon coupling is strongly enhanced for specific values of electron-momentum, k. We use inelastic neutron scattering, soft x-ray angle-resolved photoemission spectroscopy measurements and ab-initio lattice dynamical and electronic band structure calculations to demonstrate this scenario in the highly anisotropic tetragonal electron-phonon superconductor YNi2B2C. This new scenario likely applies to a wide range of compounds.

Momentum-resolved electronic structure and band offsets in an epitaxial NbN/GaN superconductor/semiconductor heterojunction.

The electronic structure of heterointerfaces is a pivotal factor for their device functionality. We use soft x-ray angle-resolved photoelectron spectroscopy to directly measure the momentum-resolved electronic band structures on both sides of the Schottky heterointerface formed by epitaxial films of the superconducting NbN on semiconducting GaN, and determine their momentum-dependent interfacial band offset as well as the band-bending profile. We find, in particular, that the Fermi states in NbN are well separated in energy and momentum from the states in GaN, excluding any notable electronic cross-talk of the superconducting states in NbN to GaN. We support the experimental findings with first-principles calculations for bulk NbN and GaN. The Schottky barrier height obtained from photoemission is corroborated by electronic transport and optical measurements. The momentum-resolved understanding of electronic properties of interfaces elucidated in our work opens up new frontiers for the quantum materials where interfacial states play a defining role.

Large linear non-saturating magnetoresistance and high mobility in ferromagnetic MnBi.

A large non-saturating magnetoresistance has been observed in several nonmagnetic topological Weyl semi-metals with high mobility of charge carriers at the Fermi energy. However, ferromagnetic systems rarely display a large magnetoresistance because of localized electrons in heavy d bands with a low Fermi velocity. Here, we report a large linear non-saturating magnetoresistance and high mobility in ferromagnetic MnBi. MnBi, unlike conventional ferromagnets, exhibits a large linear non-saturating magnetoresistance of 5000% under a pulsed field of 70 T. The electrons and holes' mobilities are both 5000 cm2V-1s-1 at 2 K, which are one of the highest for ferromagnetic materials. These phenomena are due to the spin-polarised Bi 6p band's sharp dispersion with a small effective mass. Our study provides an approach to achieve high mobility in ferromagnetic systems with a high Curie temperature, which is advantageous for topological spintronics.

Band Structure Extraction at Hybrid Narrow-Gap Semiconductor-Metal Interfaces.

The design of epitaxial semiconductor-superconductor and semiconductor-metal quantum devices requires a detailed understanding of the interfacial electronic band structure. However, the band alignment of buried interfaces is difficult to predict theoretically and to measure experimentally. This work presents a procedure that allows to reliably determine critical parameters for engineering quantum devices; band offset, band bending profile, and number of occupied quantum well subbands of interfacial accumulation layers at semiconductor-metal interfaces. Soft X-ray angle-resolved photoemission is used to directly measure the quantum well states as well as valence bands and core levels for the InAs(100)/Al interface, an important platform for Majorana-zero-mode based topological qubits, and demonstrate that the fabrication process strongly influences the band offset, which in turn controls the topological phase diagrams. Since the method is transferable to other narrow gap semiconductors, it can be used more generally for engineering semiconductor-metal and semiconductor-superconductor interfaces in gate-tunable superconducting devices.

Band-Order Anomaly at the γ-Al2O3/SrTiO3 Interface Drives the Electron-Mobility Boost.

The rich functionalities of transition-metal oxides and their interfaces bear an enormous technological potential. Its realization in practical devices requires, however, a significant improvement of yet relatively low electron mobility in oxide materials. Recently, a mobility boost of about 2 orders of magnitude has been demonstrated at the spinel-perovskite γ-Al2O3/SrTiO3 interface compared to the paradigm perovskite-perovskite LaAlO3/SrTiO3 interface. We explore the fundamental physics behind this phenomenon from direct measurements of the momentum-resolved electronic structure of this interface using resonant soft-X-ray angle-resolved photoemission. We find an anomaly in orbital ordering of the mobile electrons in γ-Al2O3/SrTiO3 which depopulates electron states in the top SrTiO3 layer. This rearrangement of the mobile electron system pushes the electron density away from the interface, which reduces its overlap with the interfacial defects and weakens the electron-phonon interaction, both effects contributing to the mobility boost. A crystal-field analysis shows that the band order alters owing to the symmetry breaking between the spinel γ-Al2O3 and perovskite SrTiO3. Band-order engineering, exploiting the fundamental symmetry properties, emerges as another route to boost the performance of oxide devices.