Emergence of quasi-1D spin-polarized states in ultrathin Bi films on InAs(111)A for spintronics applications.

The discovery, characterization, and control of heavy-fermion low-dimensional materials are central to nanoscience since quantum phenomena acquire an exotic and highly tunable character. In this work, through a variety of comprehensive experimental and theoretical techniques, it was observed and predicted that the synthesis of ultrathin Bi films on the InAs(111)A surface produces quasi-one-dimensional spin-polarized states, providing a platform for the realization of a unique spin-transport regime in the system. Scanning tunneling microscopy and low-energy electron diffraction measurements revealed that the InAs(111)A substrate facilitates the formation of the Bi-dimer phase of 2√3 × 3 periodicity with an admixture of the Bi-bilayer phase under submonolayer Bi deposition. X-ray photoelectron spectroscopy (XPS) measurements have shown the chemical stability of the Bi-induced phases, while spin and angle resolved photoemission spectroscopy (SARPES) observations combined with state-of-the-art DFT calculations have revealed that the electronic spectrum of the Bi-dimer phase holds a quasi-1D hole-like spin-split state at the Fermi level with advanced spin texture, whereas the Bi-bilayer phase demonstrates metallic states with large Rashba spin-splitting. The band structure of the Bi/InAs(111)A interface is discovered to hold great potential as a high-performance spintronics material fabricated in the ultimate two-dimensional limit.

Evolution of Mn1-xGexBi2Te4 Electronic Structure under Variation of Ge Content.

One of the approaches to manipulate MnBi2Te4 properties is the magnetic dilution, which inevitably affects the interplay of magnetism and band topology in the system. In this work, we carried out angle-resolved photoemission spectroscopy (ARPES) measurements and density functional theory (DFT) calculations for analysing changes in the electronic structure of Mn1-xGexBi2Te4 that occur under parameter x variation. We consider two ways of Mn/Ge substitution: (i) bulk doping of the whole system; (ii) surface doping of the first septuple layer. For the case (i), the experimental results reveal a decrease in the value of the bulk band gap, which should be reversed by an increase when the Ge concentration reaches a certain value. Ab-initio calculations show that at Ge concentrations above 50%, there is an absence of the bulk band inversion of the Te pz and Bi pz contributions at the Γ-point with significant spatial redistribution of the states at the band gap edges into the bulk, suggesting topological phase transition in the system. For case (ii) of the vertical heterostructure Mn1-xGexBi2Te4/MnBi2Te4, it was shown that an increase of Ge concentration in the first septuple layer leads to effective modulation of the Dirac gap in the absence of significant topological surface states of spatial redistribution. The results obtained indicate that surface doping compares favorably compared to bulk doping as a method for the Dirac gap value modulation.

Semiconducting Electronic Structure of the Ferromagnetic Spinel HgCr_{2}Se_{4} Revealed by Soft-X-Ray Angle-Resolved Photoemission Spectroscopy.

We study the electronic structure of the ferromagnetic spinel HgCr_{2}Se_{4} by soft-x-ray angle-resolved photoemission spectroscopy (SX-ARPES) and first-principles calculations. While a theoretical study has predicted that this material is a magnetic Weyl semimetal, SX-ARPES measurements give direct evidence for a semiconducting state in the ferromagnetic phase. Band calculations based on the density functional theory with hybrid functionals reproduce the experimentally determined band gap value, and the calculated band dispersion matches well with ARPES experiments. We conclude that the theoretical prediction of a Weyl semimetal state in HgCr_{2}Se_{4} underestimates the band gap, and this material is a ferromagnetic semiconductor.

Vacuum Spin LED: First Step towards Vacuum Semiconductor Spintronics.

Improving the efficiency of spin generation, injection, and detection remains a key challenge for semiconductor spintronics. Electrical injection and optical orientation are two methods of creating spin polarization in semiconductors, which traditionally require specially tailored p-n junctions, tunnel or Schottky barriers. Alternatively, we introduce here a novel concept for spin-polarized electron emission/injection combining the optocoupler principle based on vacuum spin-polarized light-emitting diode (spin VLED) making it possible to measure the free electron beam polarization injected into the III-V heterostructure with quantum wells (QWs) based on the detection of polarized cathodoluminescence (CL). To study the spin-dependent emission/injection, we developed spin VLEDs, which consist of a compact proximity-focused vacuum tube with a spin-polarized electron source (p-GaAs(Cs,O) or Na2KSb) and the spin detector (III-V heterostructure), both activated to a negative electron affinity (NEA) state. The coupling between the photon helicity and the spin angular momentum of the electrons in the photoemission and injection/detection processes is realized without using either magnetic material or a magnetic field. Spin-current detection efficiency in spin VLED is found to be 27% at room temperature. The created vacuum spin LED paves the way for optical generation and spin manipulation in the developing vacuum semiconductor spintronics.

Correction: Depth-resolved oxidational studies of Be/Al periodic multilayers investigated by X-ray photoelectron spectroscopy.

Correction for 'Depth-resolved oxidational studies of Be/Al periodic multilayers investigated by X-ray photoelectron spectroscopy' by Niranjan Kumar et al., Phys. Chem. Chem. Phys., 2023, 25, 1205-1213, https://doi.org/10.1039/D2CP04778K.

Depth-resolved oxidational studies of Be/Al periodic multilayers investigated by X-ray photoelectron spectroscopy.

The quantification of surface and subsurface oxidation of Be/Al periodic multilayer mirrors due to exposure in the ambient atmosphere was investigated by depth-resolved X-ray photoelectron spectroscopy. The contribution of oxidation was lower for the thicker layer of Al in the periodic structures since the surface was less chemically reactive for the oxidation. This was investigated by finding the depth-resolved slope of the intensity ratio of metal/oxides (Be/BeOx and Al/AlOx) by analyzing the chemical shift of Al 1s and Be 1s photoelectrons. Furthermore, a well-resolved doublet chemical shift in the O 1s spectra indicated the formation of BeOx/AlOx and BeOH/AlOH oxides. The investigation showed that the subsurface and surface regions were dominated by metal-hydroxide (BeOH/AlOH) and metal-oxide (BeOx/AlOx) bonding, respectively, analyzed by the depth-resolved chemical shifts.

Ferromagnetic Layers in a Topological Insulator (Bi,Sb)2Te3 Crystal Doped with Mn.

Magnetic topological insulators (MTIs) have recently become a subject of poignant interest; among them, Z2 topological insulators with magnetic moment ordering caused by embedded magnetic atoms attract special attention. In such systems, the case of magnetic anisotropy perpendicular to the surface that holds a topologically nontrivial surface state is the most intriguing one. Such materials demonstrate the quantum anomalous Hall effect, which manifests itself as chiral edge conduction channels that can be manipulated by switching the polarization of magnetic domains. In the present paper, we uncover the atomic structure of the bulk and the surface of Mn0.06Sb1.22Bi0.78Te3.06 in conjunction with its electronic and magnetic properties; this material is characterized by naturally formed ferromagnetic layers inside the insulating matrix, where the Fermi level is tuned to the bulk band gap. We found that in such mixed crystals septuple layers (SLs) of Mn(Bi,Sb)2Te4 form structures that feature three SLs, each of which is separated by two or three (Bi,Sb)2Te3 quintuple layers (QLs); such a structure possesses ferromagnetic properties. The surface obtained by cleavage includes terraces with different terminations. Manganese atoms preferentially occupy the central positions in the SLs and in a very small proportion can appear in the QLs, as indirectly indicated by a reshaped Dirac cone.

Electronic Structure of Pb Adsorbed Surfaces of Intrinsic Magnetic Topological Insulators.

Recently discovered intrinsic magnetic topological insulators (IMTIs) constitute a unique class of quantum materials that combine magnetism and nontrivial topology. One of the most promising applications of these materials is Majorana fermion creation; Majorana fermions are expected to arise when a superconductor is in contact with the surface of an IMTI. Here we study the adsorption of Pb ultrathin films on top of IMTIs of various stoichiometries. By means of XPS we figure out the formation of the Pb wetting layer coupled to the surface atoms for low coverages and overlayer growth on top upon further deposition. Investigation of the adsorbed surfaces by means of ARPES shows the Dirac cone survival, its shift in a binding energy, and the Pb electronic states appearance. The obtained results allow the Pb/IMTI interfaces to be constructed for the understanding of the proximity effect and provide an important step toward quantum device engineering based on IMTIs.

A volume plasmon blueshift in thin silicon films embedded within Be/Si periodic multilayer mirrors.

Microstructural properties of the beryllium (Be) and silicon (Si) in periodic multilayer mirrors Be/Si with the variation of film thickness were comprehensively determined by Raman scattering. For the thinner films, the structure of Be evolved in the amorphous phase, and it was transformed into the polycrystalline phase for thicker films. The Si films in the periodic structure were condensed into the amorphous phase. The small fraction of nanocrystalline Si particles was distributed within the amorphous phase. A shake-up satellite peak of Si 2s photoelectrons was observed in X-ray photoelectron spectroscopy which suggested the excitation of a plasmon in Si films embedded within Be/Si periodic multilayers. The energy of plasmons was sensitive to the film thickness of Si in the periods which directly corresponds to the particle size. The binding energy of the satellite peak of Si 2s photoelectrons was blueshifted (higher energy) with a decrease in the particle size. This was explained by size dependent quantum confinement of particles.

A new imaging concept in spin polarimetry based on the spin-filter effect.

The concept of an imaging-type 3D spin detector, based on the combination of spin-exchange interactions in the ferromagnetic (FM) film and spin selectivity of the electron-photon conversion effect in a semiconductor heterostructure, is proposed and demonstrated on a model system. This novel multichannel concept is based on the idea of direct transfer of a 2D spin-polarized electron distribution to image cathodoluminescence (CL). The detector is a hybrid structure consisting of a thin magnetic layer deposited on a semiconductor structure allowing measurement of the spatial and polarization-dependent CL intensity from injected spin-polarized free electrons. The idea is to use spin-dependent electron transmission through in-plane magnetized FM film for in-plane spin detection by measuring the CL intensity from recombined electrons transmitted in the semiconductor. For the incoming electrons with out-of-plane spin polarization, the intensity of circularly polarized CL light can be detected from recombined polarized electrons with holes in the semiconductor. In order to demonstrate the ability of the solid-state spin detector in the image-type mode operation, a spin detector prototype was developed, which consists of a compact proximity focused vacuum tube with a spin-polarized electron source [p-GaAs(Cs,O)], a negative electron affinity (NEA) photocathode and the target [semiconductor heterostructure with quantum wells also with NEA]. The injection of polarized low-energy electrons into the target by varying the kinetic energy in the range 0.5-3.0 eV and up to 1.3 keV was studied in image-type mode. The figure of merit as a function of electron kinetic energy and the target temperature is determined. The spin asymmetry of the CL intensity in a ferromagnetic/semiconductor (FM-SC) junction provides a compact optical method for measuring spin polarization of free-electron beams in image-type mode. The FM-SC detector has the potential for realizing multichannel 3D vectorial reconstruction of spin polarization in momentum microscope and angle-resolved photoelectron spectroscopy systems.

Correlation of elastic and optoelectronic properties near structural phase transition in organic-inorganic lead iodide perovskite single crystals.

The experimental evidence of the influence of the structural phase transition on the elastic and optoelectronic properties of CH3NH3PbI3single crystals has been reported. A peak in the attenuation for longitudinal and shear ultrasonic waves and a step-like anomaly in their velocity have been found near the structural the orthorhombic-to-tetragonal phase transition (160 K). The narrow hysteresis observed in the temperature dependences of the elastic properties confirms that this is the first-order phase transition. A redshift of the absorption threshold (of about 110 meV) has been revealed both in the photocurrent (PC) and in the photoluminescence (PL) spectra with increasing temperature from 140 to 160 K. In the orthorhombic phase of CH3NH3PbI3single crystals, the fine exciton structure in the PC spectrum has been found with an exciton binding energy of 19-25 meV. The peculiarities of the PC and PL spectra near the phase transition temperature (160 K) have been observed within a wider temperature range in contrast to the elastic anomalies that can be explained by the complex structure of the near-surface region. It may be essential for the further development of optoelectronic devices based on hybrid halide perovskites.

Topologically Nontrivial Phase-Change Compound GeSb2Te4.

Chalcogenide phase-change materials show strikingly contrasting optical and electrical properties, which has led to their extensive implementation in various memory devices. By performing spin-, time-, and angle-resolved photoemission spectroscopy combined with the first-principles calculation, we report the experimental results that the crystalline phase of GeSb2Te4 is topologically nontrivial in the vicinity of the Dirac semimetal phase. The resulting linearly dispersive bulk Dirac-like bands that cross the Fermi level and are thus responsible for conductivity in the stable crystalline phase of GeSb2Te4 can be viewed as a 3D analogue of graphene. Our finding provides us with the possibility of realizing inertia-free Dirac currents in phase-change materials.

Shubnikov-de Haas oscillations in p and n-type topological insulator (Bi x Sb1-x )2Te3.

We show Shubnikov-de Haas (SdH) oscillations in topological insulator (Bi x Sb1-x )2Te3 flakes whose carrier types are p-type (x = 0.29, 0.34) and n-type (x = 0.42). The physical properties such as the Berry phase, carrier mobility, and scattering time significantly changed by tuning the Fermi-level position with the concentration x. The analyses of SdH oscillations by Landau-level fan diagram, Lifshitz-Kosevich theory, and Dingle-plot in the p-type samples with x = 0.29 and 0.34 showed the Berry phase of zero and a relatively low mobility (2000-6000 cm2 V-1 s-1). This is due to the dominant bulk component in transport. On the other hand, the mobility in the n-type sample with x = 0.42 reached a very large value ~17 000 cm2 V-1 s-1 and the Berry phase of near π, whereas the SdH oscillations were neither purely two- nor three-dimensional. These suggest that the transport channel has a surface-bulk coupling state which makes the carrier scattering lesser and enhances the mobility and has a character between two- and three-dimension.

Dual nature of magnetic dopants and competing trends in topological insulators.

Topological insulators interacting with magnetic impurities have been reported to host several unconventional effects. These phenomena are described within the framework of gapping Dirac quasiparticles due to broken time-reversal symmetry. However, the overwhelming majority of studies demonstrate the presence of a finite density of states near the Dirac point even once topological insulators become magnetic. Here, we map the response of topological states to magnetic impurities at the atomic scale. We demonstrate that magnetic order and gapless states can coexist. We show how this is the result of the delicate balance between two opposite trends, that is, gap opening and emergence of a Dirac node impurity band, both induced by the magnetic dopants. Our results evidence a more intricate and rich scenario with respect to the once generally assumed, showing how different electronic and magnetic states may be generated and controlled in this fascinating class of materials.

Spin-texture inversion in the giant Rashba semiconductor BiTeI.

Semiconductors with strong spin-orbit interaction as the underlying mechanism for the generation of spin-polarized electrons are showing potential for applications in spintronic devices. Unveiling the full spin texture in momentum space for such materials and its relation to the microscopic structure of the electronic wave functions is experimentally challenging and yet essential for exploiting spin-orbit effects for spin manipulation. Here we employ a state-of-the-art photoelectron momentum microscope with a multichannel spin filter to directly image the spin texture of the layered polar semiconductor BiTeI within the full two-dimensional momentum plane. Our experimental results, supported by relativistic ab initio calculations, demonstrate that the valence and conduction band electrons in BiTeI have spin textures of opposite chirality and of pronounced orbital dependence beyond the standard Rashba model, the latter giving rise to strong optical selection-rule effects on the photoelectron spin polarization. These observations open avenues for spin-texture manipulation by atomic-layer and charge carrier control in polar semiconductors.

Plasma-Wave Terahertz Detection Mediated by Topological Insulators Surface States.

Topological insulators (TIs) represent a novel quantum state of matter, characterized by edge or surface-states, showing up on the topological character of the bulk wave functions. Allowing electrons to move along their surface, but not through their inside, they emerged as an intriguing material platform for the exploration of exotic physical phenomena, somehow resembling the graphene Dirac-cone physics, as well as for exciting applications in optoelectronics, spintronics, nanoscience, low-power electronics, and quantum computing. Investigation of topological surface states (TSS) is conventionally hindered by the fact that in most of experimental conditions the TSS properties are mixed up with those of bulk-states. Here, we activate, probe, and exploit the collective electronic excitation of TSS in the Dirac cone. By engineering Bi2Te(3-x)Sex stoichiometry, and by gating the surface of nanoscale field-effect-transistors, exploiting thin flakes of Bi2Te2.2Se0.8 or Bi2Se3, we provide the first demonstration of room-temperature terahertz (THz) detection mediated by overdamped plasma-wave oscillations on the "activated" TSS of a Bi2Te2.2Se0.8 flake. The reported detection performances allow a realistic exploitation of TSS for large-area, fast imaging, promising superb impacts on THz photonics.

Signatures of Dirac fermion-mediated magnetic order.

The spin-momentum locking of topological states offers an ideal platform to explore novel magnetoelectric effects. These intimately depend on the ability to manipulate the spin texture in a controlled way. Here we combine scanning tunnelling microscopy with single-atom deposition to map the evolution of topological states under the influence of different magnetic perturbations. We obtain signatures of Dirac fermion-mediated magnetic order for extremely dilute adatom concentrations. This striking observation is found to critically depend on the single adatoms' magnetic anisotropy and the position of the Fermi level. Our findings open new perspectives in spin engineering topological states at the atomic scale and pave the way to explore novel spin-related topological phenomena with promising potential for applications.