Electronic Band Structure Changes across the Antiferromagnetic Phase Transition of Exfoliated MnPS3 Flakes Probed by µ-ARPES.

Exfoliated magnetic 2D materials enable versatile tuning of magnetization, e.g., by gating or providing proximity-induced exchange interaction. However, their electronic band structure after exfoliation has not been probed, presumably due to their photochemical sensitivity. Here, we provide micrometer-scale angle-resolved photoelectron spectroscopy of the exfoliated intralayer antiferromagnet MnPS3 above and below the Néel temperature down to one monolayer. Favorable comparison with density functional theory calculations enables identifying the orbital character of the observed bands. Consistently, we find pronounced changes across the Néel temperature for bands consisting of Mn 3d and 3p levels of adjacent S atoms. The deduced orbital mixture indicates that the superexchange is relevant for the magnetic interaction. There are only minor changes between monolayer and thicker films, demonstrating the predominant 2D character of MnPS3. The novel access is transferable to other MPX3 materials (M: transition metal, P: phosphorus, X: chalcogenide), providing several antiferromagnetic arrangements.

Geometry-Induced Spin Filtering in Photoemission Maps from WTe_{2} Surface States.

We demonstrate that an important quantum material WTe_{2} exhibits a new type of geometry-induced spin filtering effect in photoemission, stemming from low symmetry that is responsible for its exotic transport properties. Through the laser-driven spin-polarized angle-resolved photoemission Fermi surface mapping, we showcase highly asymmetric spin textures of electrons photoemitted from the surface states of WTe_{2}. Such asymmetries are not present in the initial state spin textures, which are bound by the time-reversal and crystal lattice mirror plane symmetries. The findings are reproduced qualitatively by theoretical modeling within the one-step model photoemission formalism. The effect could be understood within the free-electron final state model as an interference due to emission from different atomic sites. The observed effect is a manifestation of time-reversal symmetry breaking of the initial state in the photoemission process, and as such it cannot be eliminated, but only its magnitude influenced, by special experimental geometries.

Direct Observation of the Band Gap Transition in Atomically Thin ReS2.

ReS2 is considered as a promising candidate for novel electronic and sensor applications. The low crystal symmetry of this van der Waals compound leads to a highly anisotropic optical, vibrational, and transport behavior. However, the details of the electronic band structure of this fascinating material are still largely unexplored. We present a momentum-resolved study of the electronic structure of monolayer, bilayer, and bulk ReS2 using k-space photoemission microscopy in combination with first-principles calculations. We demonstrate that the valence electrons in bulk ReS2 are-contrary to assumptions in recent literature-significantly delocalized across the van der Waals gap. Furthermore, we directly observe the evolution of the valence band dispersion as a function of the number of layers, revealing the transition from an indirect band gap in bulk ReS2 to a direct gap in the bilayer and the monolayer. We also find a significantly increased effective hole mass in single-layer crystals. Our results establish bilayer ReS2 as an advantageous building block for two-dimensional devices and van der Waals heterostructures.

Phase-Selective Epitaxy of Trigonal and Orthorhombic Bismuth Thin Films on Si (111).

Over the past three decades, the growth of Bi thin films has been extensively explored due to their potential applications in various fields such as thermoelectrics, ferroelectrics, and recently for topological and neuromorphic applications, too. Despite significant research efforts in these areas, achieving reliable and controllable growth of high-quality Bi thin-film allotropes has remained a challenge. Previous studies have reported the growth of trigonal and orthorhombic phases on various substrates yielding low-quality epilayers characterized by surface morphology. In this study, we present a systematic growth investigation, enabling the high-quality growth of Bi epilayers on Bi-terminated Si (111) 1 × 1 surfaces using molecular beam epitaxy. Our work yields a phase map that demonstrates the realization of trigonal, orthorhombic, and pseudocubic thin-film allotropes of Bi. In-depth characterization through X-ray diffraction (XRD) techniques and scanning transmission electron microscopy (STEM) analysis provides a comprehensive understanding of phase segregation, phase stability, phase transformation, and phase-dependent thickness limitations in various Bi thin-film allotropes. Our study provides recipes for the realization of high-quality Bi thin films with desired phases, offering opportunities for the scalable refinement of Bi into quantum and neuromorphic devices and for revisiting technological proposals for this versatile material platform from the past 30 years.

Mixed topological semimetals driven by orbital complexity in two-dimensional ferromagnets.

The concepts of Weyl fermions and topological semimetals emerging in three-dimensional momentum space are extensively explored owing to the vast variety of exotic properties that they give rise to. On the other hand, very little is known about semimetallic states emerging in two-dimensional magnetic materials, which present the foundation for both present and future information technology. Here, we demonstrate that including the magnetization direction into the topological analysis allows for a natural classification of topological semimetallic states that manifest in two-dimensional ferromagnets as a result of the interplay between spin-orbit and exchange interactions. We explore the emergence and stability of such mixed topological semimetals in realistic materials, and point out the perspectives of mixed topological states for current-induced orbital magnetism and current-induced domain wall motion. Our findings pave the way to understanding, engineering and utilizing topological semimetallic states in two-dimensional spin-orbit ferromagnets.

Environmental Control of Charge Density Wave Order in Monolayer 2H-TaS2.

For quasi-freestanding 2H-TaS2 in monolayer thickness grown by in situ molecular beam epitaxy on graphene on Ir(111), we find unambiguous evidence for a charge density wave close to a 3 × 3 periodicity. Using scanning tunneling spectroscopy, we determine the magnitude of the partial charge density wave gap. Angle-resolved photoemission spectroscopy, complemented by scanning tunneling spectroscopy for the unoccupied states, makes a tight-binding fit for the band structure of the TaS2 monolayer possible. As hybridization with substrate bands is absent, the fit yields a precise value for the doping of the TaS2 layer. Additional Li doping shifts the charge density wave to a 2 × 2 periodicity. Unexpectedly, the bilayer of TaS2 also displays a disordered 2 × 2 charge density wave. Calculations of the phonon dispersions based on a combination of density-functional theory, density-functional perturbation theory, and many-body perturbation theory enable us to provide phase diagrams for the TaS2 charge density wave as functions of doping, hybridization, and interlayer potentials, and offer insight into how they affect lattice dynamics and stability. Our theoretical considerations are consistent with the experimental work presented and shed light on previous experimental and theoretical investigations of related systems.

Element- and momentum-resolved electronic structure of the dilute magnetic semiconductor manganese doped gallium arsenide.

The dilute magnetic semiconductors have promise in spin-based electronics applications due to their potential for ferromagnetic order at room temperature, and various unique switching and spin-dependent conductivity properties. However, the precise mechanism by which the transition-metal doping produces ferromagnetism has been controversial. Here we have studied a dilute magnetic semiconductor (5% manganese-doped gallium arsenide) with Bragg-reflection standing-wave hard X-ray angle-resolved photoemission spectroscopy, and resolved its electronic structure into element- and momentum- resolved components. The measured valence band intensities have been projected into element-resolved components using analogous energy scans of Ga 3d, Mn 2p, and As 3d core levels, with results in excellent agreement with element-projected Bloch spectral functions and clarification of the electronic structure of this prototypical material. This technique should be broadly applicable to other multi-element materials.

Bi1Te1 is a dual topological insulator.

New three-dimensional (3D) topological phases can emerge in superlattices containing constituents of known two-dimensional topologies. Here we demonstrate that stoichiometric Bi1Te1, which is a natural superlattice of alternating two Bi2Te3 quintuple layers and one Bi bilayer, is a dual 3D topological insulator where a weak topological insulator phase and topological crystalline insulator phase appear simultaneously. By density functional theory, we find indices (0;001) and a non-zero mirror Chern number. We have synthesized Bi1Te1 by molecular beam epitaxy and found evidence for its topological crystalline and weak topological character by spin- and angle-resolved photoemission spectroscopy. The dual topology opens the possibility to gap the differently protected metallic surface states on different surfaces independently by breaking the respective symmetries, for example, by magnetic field on one surface and by strain on another surface.

Electrical resistance of individual defects at a topological insulator surface.

Three-dimensional topological insulators host surface states with linear dispersion, which manifest as a Dirac cone. Nanoscale transport measurements provide direct access to the transport properties of the Dirac cone in real space and allow the detailed investigation of charge carrier scattering. Here we use scanning tunnelling potentiometry to analyse the resistance of different kinds of defects at the surface of a (Bi0.53Sb0.47)2Te3 topological insulator thin film. We find the largest localized voltage drop to be located at domain boundaries in the topological insulator film, with a resistivity about four times higher than that of a step edge. Furthermore, we resolve resistivity dipoles located around nanoscale voids in the sample surface. The influence of such defects on the resistance of the topological surface state is analysed by means of a resistor network model. The effect resulting from the voids is found to be small compared with the other defects.

Band structure evolution during the ultrafast ferromagnetic-paramagnetic phase transition in cobalt.

The evolution of the electronic band structure of the simple ferromagnets Fe, Co, and Ni during their well-known ferromagnetic-paramagnetic phase transition has been under debate for decades, with no clear and even contradicting experimental observations so far. Using time- and spin-resolved photoelectron spectroscopy, we can make a movie on how the electronic properties change in real time after excitation with an ultrashort laser pulse. This allows us to monitor large transient changes in the spin-resolved electronic band structure of cobalt for the first time. We show that the loss of magnetization is not only found around the Fermi level, where the states are affected by the laser excitation, but also reaches much deeper into the electronic bands. We find that the ferromagnetic-paramagnetic phase transition cannot be explained by a loss of the exchange splitting of the spin-polarized bands but instead shows rapid band mirroring after the excitation, which is a clear signature of extremely efficient ultrafast magnon generation. Our result helps to understand band structure formation in these seemingly simple ferromagnetic systems and gives first clear evidence of the transient processes relevant to femtosecond demagnetization.

Quasi 2D electronic states with high spin-polarization in centrosymmetric MoS2 bulk crystals.

Time reversal dictates that nonmagnetic, centrosymmetric crystals cannot be spin-polarized as a whole. However, it has been recently shown that the electronic structure in these crystals can in fact show regions of high spin-polarization, as long as it is probed locally in real and in reciprocal space. In this article we present the first observation of this type of compensated polarization in MoS2 bulk crystals. Using spin- and angle-resolved photoemission spectroscopy (ARPES), we directly observed a spin-polarization of more than 65% for distinct valleys in the electronic band structure. By additionally evaluating the probing depth of our method, we find that these valence band states at the point in the Brillouin zone are close to fully polarized for the individual atomic trilayers of MoS2, which is confirmed by our density functional theory calculations. Furthermore, we show that this spin-layer locking leads to the observation of highly spin-polarized bands in ARPES since these states are almost completely confined within two dimensions. Our findings prove that these highly desired properties of MoS2 can be accessed without thinning it down to the monolayer limit.

Realization of a vertical topological p-n junction in epitaxial Sb2Te3/Bi2Te3 heterostructures.

Three-dimensional (3D) topological insulators are a new state of quantum matter, which exhibits both a bulk band structure with an insulating energy gap as well as metallic spin-polarized Dirac fermion states when interfaced with a topologically trivial material. There have been various attempts to tune the Dirac point to a desired energetic position for exploring its unusual quantum properties. Here we show a direct experimental proof by angle-resolved photoemission of the realization of a vertical topological p-n junction made of a heterostructure of two different binary 3D TI materials Bi2Te3 and Sb2Te3 epitaxially grown on Si(111). We demonstrate that the chemical potential is tunable by about 200 meV when decreasing the upper Sb2Te3 layer thickness from 25 to 6 quintuple layers without applying any external bias. These results make it realistic to observe the topological exciton condensate and pave the way for exploring other exotic quantum phenomena in the near future.

Quantized electron accumulation states in indium nitride studied by angle-resolved photoemission spectroscopy.

Electron accumulation states in InN have been measured using high resolution angle-resolved photoemission spectroscopy (ARPES). The electrons in the accumulation layer have been discovered to reside in quantum well states. ARPES was also used to measure the Fermi surface of these quantum well states, as well as their constant binding energy contours below the Fermi level E(F). The energy of the Fermi level and the size of the Fermi surface for these quantum well states could be controlled by varying the method of surface preparation. This is the first unambiguous observation that electrons in the InN accumulation layer are quantized and the first time the Fermi surface associated with such states has been measured.