Angle-resolved Photoemission Spectroscopy Results Research Articles

Observation of highly anisotropic bulk dispersion and spin-polarized topological surface states in CoTe2

We present CoTe2 as a new type-II Dirac semimetal supporting Lorentz symmetry violating Dirac fermions in the vicinity of the Fermi energy. By combining first principle ab-initio calculations with experimental angle-resolved photo-emission spectroscopy results, we show the CoTe2 hosts a pair of type-II Dirac fermions around 90 meV above the Fermi energy. In addition to the bulk Dirac fermions, we find several topological band inversions in bulk CoTe2, which gives rise to a ladder of spin-polarized surface states over a wide range of energies. In contrast to the surface states which typically display Rashba-type in-plane spin splitting, we find that CoTe2 hosts novel out-of-plane spin polarization as well. Our work establishes CoTe2 as a potential candidate for the exploration of Dirac fermiology and applications in spintronic devices, infrared plasmonics, and ultrafast optoelectronics.

Role of Hollow Defects in Lattice Phase Separation and Electronic Features in Quasi-One-Dimensional Bi4I4 Crystals

The defects play a crucial role in the determination of the crystal structure and electronic properties of the matter, evoking tremendous interest in the manipulation of defects and exploration of underlying mechanisms. In this work, we applied scanning tunneling microscopy to investigate the influence of the defects on the lattice structure and electronic properties of Bi4I4 crystals. A lattice phase separation in the nanoscale is identified in the vicinity of hollow defects, which is absent in the sample without defects. The scanning tunneling spectroscopy reveals a bandgap around 0.1 eV at the terrace of (001) surface of Bi4I4, which is consistent with the angle-resolved photoemission spectroscopy results and first-principles calculations. The hollow defects modulate the local density of the state, leading to the edge state residing in the gap region. This edge state is regarded as responsible for the varied resistivity in different Bi4I4 samples in previous reports as their densities of the hollow defects are diverse. Our results shed light on the argument over the lattice phase of Bi4I4 at low temperatures as well as the factors determining the electronic properties.

Competing magnetic and nonmagnetic states in monolayer VSe2 with charge density wave

The field of two-dimensional ferromagnets has been reinvigorated by the discovery of ${\mathrm{VSe}}_{2}$ monolayer grown on van der Waals substrates, which is reported to be ferromagnetic with a Curie point higher than 330 K. However, the ferromagnetic and nonmagnetic states of pristine monolayer ${\mathrm{VSe}}_{2}$ are highly debated. Here, employing density functional theory, Wannier function calculations, and the band unfolding method, we explore the electronic structure of monolayer ${\mathrm{VSe}}_{2}$ with a $\sqrt{3}\ifmmode\times\else\texttimes\fi{}\sqrt{7}$ charge density wave (CDW). Certain qualitative aspects of the calculated unfolded band dispersion and unfolded Fermi surface of monolayer ${\mathrm{VSe}}_{2}$ with the $\sqrt{3}\ifmmode\times\else\texttimes\fi{}\sqrt{7}$ CDW in the nonmagnetic state agree well with previous angle-resolved photoemission spectroscopy results, albeit with uncertainty about whether these experiments probed single or multiple domains. Specifically, we find that an isolated CDW domain naturally induces a strong breaking of the threefold symmetry of the electronic structure. In addition we find that, relative to the undistorted structure, the CDW structure shows a strong competition between nonmagnetic and various magnetic states, with an energy difference less than 5 meV/f.u. For the CDW structure in the antiferromagnetic state, the band dispersions and Fermi surface are similar to those in the nonmagnetic state, while the unfolded bands of the ferromagnetic CDW state display a sizable exchange splitting. These results indicate the possibility of various antiferromagnetic fluctuations in ${\mathrm{VSe}}_{2}$ to coexist and compete with ferromagnetic order and the experimentally reported CDW order. Our calculations build insights for exploring the interplay between magnetism and CDW behaviors more generally in transition metal dichalcogenides.

Electronic Structure of InAs and InSb Surfaces: Density Functional Theory and Angle‐Resolved Photoemission Spectroscopy

AbstractThe electronic structure of surfaces plays a key role in the properties of quantum devices. However, surfaces are also the most challenging to simulate and engineer. Here, the electronic structure of InAs(001), InAs(111), and InSb(110) surfaces is studied using a combination of density functional theory (DFT) and angle‐resolved photoemission spectroscopy (ARPES). Large‐scale first principles simulations are enabled by using DFT calculations with a machine‐learned Hubbard U correction [npj Comput. Mater. 6, 180 (2020)]. To facilitate direct comparison with ARPES results, a “bulk unfolding” scheme is implemented by projecting the calculated band structure of a supercell surface slab model onto the bulk primitive cell. For all three surfaces, a good agreement is found between DFT calculations and ARPES. For InAs(001), the simulations clarify the effect of the surface reconstruction. Different reconstructions are found to produce distinctive surface states, which may be detected by ARPES with low photon energies. For InAs(111) and InSb(110), the simulations help elucidate the effect of oxidation. Owing to larger charge transfer from As to O than from Sb to O, oxidation of InAs(111) leads to significant band bending and produces an electron pocket, whereas oxidation of InSb(110) does not. The combined theoretical and experimental results may inform the design of quantum devices based on InAs and InSb semiconductors, for example, topological qubits utilizing the Majorana zero modes.

Fermiology of two-dimensional titanium carbide and nitride MXenes

MXenes are a family two-dimensional transition-metal carbide and nitride materials, which often exhibit very good metallic conductivity and are thus of great interest for applications in, e.g., flexible electronics, electrocatalysis, and electromagnetic interference shielding. However, surprisingly little is known about the fermiology of MXenes, i.e., the shape and size of their Fermi surfaces, and its effect on the material properties. One reason for this may be that MXene surfaces are almost always covered by a mixture of functional groups, and studying Fermi surfaces of disordered systems is cumbersome. Here, we study fermiology of four common Ti-based MXenes as a function of the surface functional group composition. We first calculate the effective band structures of systems with explicit mixed surfaces and observe gradual evolution in the filling of the Ti-d band and resulting shift of Fermi level. We then demonstrate that these band structures can be closely approximated by using pseudohydrogenated surfaces, and also compare favorably to the experimental angle-resolved photoemission spectroscopy results. By modifying the pseudohydrogen charge we then proceed to plot Fermi surfaces for all systems and extract their properties, such as the Fermi-surface area and average Fermi velocity. These are in turn used to evaluate the electrical conductivity with the relaxation time fitted to experimentally measured conductivities.

Two-dimensional Dirac dispersion in the layered compound BaCdSb2

We report a comprehensive study of the electronic structure of layered compound $\mathrm{Ba}\mathrm{Cd}{\mathrm{Sb}}_{2}$ by using electrical transport measurements, first-principles calculations, and angle-resolved photoemission spectroscopy (ARPES). The samples show semiconductorlike temperature dependence of resistivity and low carrier density. The Shubnikov-de Haas (SdH) oscillations with a single frequency reveal a small two-dimensional (2D) cylinderlike Fermi surface (FS), a light cyclotron effective mass, and trivial Berry's phase. Quantum limit can be achieved under a moderate magnetic field. The calculated bands without any renormalization are well consistent with the ARPES results, showing the Dirac band crossing with 2D character near the Fermi energy and a gap of about 34 meV at the Dirac point induced by spin-orbit interaction. The SdH oscillations can be identified to the Dirac band by the similar cross sectional areas of FSs. Our findings indicate $\mathrm{Ba}\mathrm{Cd}{\mathrm{Sb}}_{2}$ is a promising material for researching the quantum phenomena of the 2D Dirac fermions.

Evolution of the Kondo lattice electronic structure above the transport coherence temperature

The temperature-dependent evolution of the Kondo lattice is a long-standing topic of theoretical and experimental investigation and yet it lacks a truly microscopic description of the relation of the basic f-c hybridization processes to the fundamental temperature scales of Kondo screening and Fermi-liquid lattice coherence. Here, the temperature dependence of f-c hybridized band dispersions and Fermi-energy f spectral weight in the Kondo lattice system CeCoIn5 is investigated using f-resonant angle-resolved photoemission spectroscopy (ARPES) with sufficient detail to allow direct comparison to first-principles dynamical mean-field theory (DMFT) calculations containing full realism of crystalline electric-field states. The ARPES results, for two orthogonal (001) and (100) cleaved surfaces and three different f-c hybridization configurations, with additional microscopic insight provided by DMFT, reveal f participation in the Fermi surface at temperatures much higher than the lattice coherence temperature, [Formula: see text] K, commonly believed to be the onset for such behavior. The DMFT results show the role of crystalline electric-field (CEF) splittings in this behavior and a T-dependent CEF degeneracy crossover below [Formula: see text] is specifically highlighted. A recent ARPES report of low T Luttinger theorem failure for CeCoIn5 is shown to be unjustified by current ARPES data and is not found in the theory.

Reversible Potassium Intercalation in Blue Phosphorene-Au Network Driven by an Electric Field.

Foreign atom intercalation into an interface alters the strength of interlayer interaction and leads to the novel types of desirable properties. Here, we report an investigation via scanning tunnelling microscopy (STM) and scanning tunnelling spectroscopy (STS) of reversible potassium (K) intercalation in the blue phosphorene (blueP)-Au network that can be locally induced by an external electric field. The unique structure of the blueP-Au network provides large space in its pores for the intercalation and deintercalation process. The X-ray photoemission spectroscopy results reveal that the intercalated K atoms are bonded with Au atoms in substrate, which weakens the interaction between the blueP-Au network and Au(111). The STS and angle-resolved photoemission spectroscopy results indicate that the electronic properties of the blueP-Au network have been modulated after the K intercalation. Such reversible intercalation and deintercalation transitions in the blueP-Au network are relevant for the design of the nanoelectronic devices as well as for its application in K-ion batteries.

Direct insight into the band structure of SrNbO3

We present the results of a photon energy and polarization dependent angle-resolved photoemission spectroscopy (ARPES) study on high quality, epitaxial ${\mathrm{SrNbO}}_{3}$ thin films prepared in situ by pulsed laser deposition (PLD). We show that the Fermi surface is composed of three bands mainly due to ${\mathrm{t}}_{2g}$ orbitals of Nb $4d$, in analogy with the $3d$-based perovskite systems. The bulk band dispersion for the conduction and valence states obtained by density functional theory (DFT) is generally consistent with the ARPES data. The small discrepancy in the bandwidth close to the Fermi level seems to result from the interplay of correlation effects and the presence of vacancies. The ARPES results are complemented by soft x-ray photoemission spectroscopy measurements in order to provide indications on the chemical states and the stoichiometry of the material.

Surface superconductivity in the type II Weyl semimetal TaIrTe4.

The search for unconventional superconductivity in Weyl semimetal materials is currently an exciting pursuit, since such superconducting phases could potentially be topologically non-trivial and host exotic Majorana modes. The layered material TaIrTe4 is a newly predicted time-reversal invariant type II Weyl semimetal with the minimum number of Weyl points. Here, we report the discovery of surface superconductivity in Weyl semimetal TaIrTe4. Our scanning tunneling microscopy/spectroscopy (STM/STS) visualizes Fermi arc surface states of TaIrTe4 that are consistent with the previous angle-resolved photoemission spectroscopy results. By a systematic study based on STS at ultralow temperature, we observe uniform superconducting gaps on the sample surface. The superconductivity is further confirmed by electrical transport measurements at ultralow temperature, with an onset transition temperature (Tc) up to 1.54 K being observed. The normalized upper critical field h*(T/Tc) behavior and the stability of the superconductivity against the ferromagnet indicate that the discovered superconductivity is unconventional with the p-wave pairing. The systematic STS, and thickness- and angular-dependent transport measurements reveal that the detected superconductivity is quasi-1D and occurs in the surface states. The discovery of the surface superconductivity in TaIrTe4 provides a new novel platform to explore topological superconductivity and Majorana modes.

Monolayer VTe2 : Incommensurate Fermi surface nesting and suppression of charge density waves

We investigated the electronic structure of monolayer VTe2 grown on bilayer graphene by angle-resolved photoemission spectroscopy (ARPES). We found that monolayer VTe2 takes the octahedral 1T structure in contrast to the monoclinic one in the bulk, as evidenced by the good agreement in the Fermi-surface topology between ARPES results and first-principles band calculations for octahedral monolayer 1T-VTe2. We have revealed that monolayer 1T-VTe2 at low temperature is characterized by a metallic state whereas the nesting condition is better than that of isostructural monolayer VSe2 which undergoes a CDW transition to insulator at low temperature. The present result suggests an importance of Fermi-surface topology for characterizing the CDW properties of monolayer TMDs.

Layer k -projection and unfolding electronic bands at interfaces

The k-projection method provides an approach to separate the contributions from different constituents in heterostructure systems and can act as an aid to connect the results of experiments and calculations. We show that the technique can be used to "unfold" the calculated electronic bands of interfaces and supercells, and provide local band structure by integrating the projected states over specified regions of space, a step that can be implemented efficiently using fast Fourier transforms. We apply the method to investigate the effects of interfaces in heterostructures consisting of a graphene bilayer on H-saturated SiC(0001), BAs monolayer on the ferromagnetic semiconductor CrI3, silicene on Ag(111), and to the Bi2Se3 surface. Our results reveal that the band structure of the graphene bilayer around the Dirac point is strongly dependent on the termination of SiC(0001): on the C face, the graphene is n doped and a gap of ~0.13 eV is opened, whereas, on the Si face, the graphene is essentially unchanged and neutral. We show that for BAs/CrI3, the magnetic proximity effect can effectively induce a spin splitting up to about 50 meV in BAs. For silicene/Ag(111), our calculations reproduce the angle-resolved photoemission spectroscopy results, including linearly dispersing bands at the edge of the first Brillouin zone of Ag(111); although these states result from the interaction between the silicene overlayer and the substrate, we demonstrate that they are not Dirac states.

Orbital-dependent band renormalization in WTe2 revealed by angle-resolved photoemission spectroscopy

The effect of electronic correlation on $\mathrm{WT}{\mathrm{e}}_{2}$ has been investigated by means of angle-resolved photoemission spectroscopy (ARPES) and band-structure calculation. In the ARPES results, the valence band top with Te $5p$ character reaches the Fermi level and forms complicated hole pockets around the zone center. In addition, two electron pockets are observed besides the hole pockets. The position of the electron pockets is inconsistent with the prediction of band calculation, suggesting the importance of electronic correlation in $\mathrm{WT}{\mathrm{e}}_{2}$. The present analysis indicates the correlation effect is associated with the excitonic coupling between the W $5d$ electron and Te $5p$ hole bands.

Weak antilocalization effect in exfoliated black phosphorus revealed by temperature- and angle-dependent magnetoconductivity

Recently, there have increasingly been debates on whether there exists a surface resonance state (SRS) in black phosphorus (BP), as suggested by recent angle-resolved photoemission spectroscopy results. To resolve this issue, we have performed temperature- and angle-dependent magnetoconductivity measurements on exfoliated, high-quality BP single crystals. A pronounced weak-antilocalization (WAL) effect was observed within a narrow temperature range of 8–16 K, with the electrical current flowing parallel to the cleaved ac-plane (along the a- or c-axis) and the magnetic field along the b-axis. The angle-dependent magnetoconductivity and the Hikami–Larkin–Nagaoka model-fitted results have revealed that the observed WAL effect shows surface-bulk coherent features, which supports the existence of SRS in BP.

Electronic properties of topological insulator candidate CaAgAs

The topological phases of matter provide the opportunity to observe many exotic properties, such as the existence of 2D topological surface states in the form of Dirac cones in topological insulators and chiral transport through the open Fermi arc in Weyl semimetals. However, these properties affect the transport characteristics and, therefore, may be useful for applications only if the topological phenomena occur near the Fermi level. CaAgAs is a promising candidate for which the ab initio calculations predict line-nodes at the Fermi energy. However, the compound transforms into a topological insulator on considering spin–orbit interaction. In this study, we investigated the electronic structure of CaAgAs with angle-resolved photoemission spectroscopy (ARPES), ab initio calculations, and transport measurements. The results from ARPES show that the bulk valence band crosses the Fermi energy at the Γ-point. The measured band dispersion matches the ab initio calculations closely when shifting the Fermi energy in the calculations by −0.5 eV. The ARPES results are in good agreement with transport measurements, which show abundant p-type carriers.

Effects of magnetic dopants in (Li0.8M0.2OH)FeSe ( M=Fe , Mn, Co): Density functional theory study using a band unfolding technique

The effects of Fe dopants in (Li$_{0.8}$Fe$_{0.2}$OH)FeSe on the electronic band structure are investigated by band unfolding ($k$-projection) technique based on first-principles supercell calculations. Doping 20\% Fe into the LiOH layers has significant effects on the band structure, that is, the Fe impurities doping electrons to the FeSe layers not only shift the Fermi level, but also induce substantial changes in the profile of bands around the Fermi level. However, the magnetic ordering in the dopants has minor effects on the band structure due to the fact that there is only a weak bonding between the LiOH and FeSe layers. Electronic bands for the surface FeSe layer show noticeable differences from those for inner layers in both the location of the Fermi level and details of the bands near the high symmetry points. The band structure for the surface FeSe layer where the Fe atoms are in checkerboard antiferromagnetic order is consistent with angle-resolved photoemission spectroscopy results. Mn and Co have similar doping effects on the band structure of (LiOH)FeSe.

Charge density waves and the Coulomb correlation effects in Na2Ti2P2O ( P=Sb,As)

To explore the origin of the phase transitions in ${\mathrm{Na}}_{2}{\mathrm{Ti}}_{2}{P}_{2}\mathrm{O}$ ($P$ = Sb, As), we have investigated their band structures and phonon dispersions based on the $ab\phantom{\rule{4pt}{0ex}}initio$ density functional theory. We have found that the phonon softening instabilities occur for both compounds at q${}_{X}$ and q${}_{M}$, which lead to charge density wave (CDW) instabilities through the electron-phonon coupling. When the Coulomb correlation effect of Ti $d$ electrons is taken into account, the CDW transition to a $2\ifmmode\times\else\texttimes\fi{}1\ifmmode\times\else\texttimes\fi{}1$ supercell driven by the normal mode at q${}_{X}$ produces the most stable state for both compounds. In the CDW ground states, ${\mathrm{Na}}_{2}{\mathrm{Ti}}_{2}{\mathrm{Sb}}_{2}\mathrm{O}$ and ${\mathrm{Na}}_{2}{\mathrm{Ti}}_{2}{\mathrm{As}}_{2}\mathrm{O}$ have the partial and full gap openings in the band structures, respectively, which are in good agreement with the observed transport and angle-resolved photoemission spectroscopy results. Our paper reveals that the Coulomb correlation effects of Ti $d$ electrons are essential to properly describe the CDW transitions in ${\mathrm{Na}}_{2}{\mathrm{Ti}}_{2}{P}_{2}\mathrm{O}$.

Electron-phonon coupling in topological surface states: The role of polar optical modes

The use of topological edge states for spintronic applications could be severely hampered by limited lifetimes due to intrinsic many-body interactions, in particular electron-phonon coupling. Previous works to determine the intrinsic coupling strength did not provide a coherent answer. Here, the electron-phonon interaction in the metallic surface state of 3D topological insulators is revised within a first principles framework. For the archetypical cases of Bi2Se3 and Bi2Te3, we find an overall weak coupling constant of less than 0.15, but with a characteristic energy dependence. Derived electronic self-energies compare favorably with previous angle-resolved photoemission spectroscopy results. The prevailing coupling is carried by optical modes of polar character, which is weakly screened by the metallic surface state and can be reduced by doping into bulk bands. We do not find any indication of a strong coupling to the A1g mode or the presence of a Kohn anomaly in the surface phonon spectrum. The weak intrinsic electron-phonon coupling guarantees long-lived quasiparticles at elevated temperatures.

Band splitting and Weyl nodes in trigonal tellurium studied by angle-resolved photoemission spectroscopy and density functional theory

We have performed high-resolution angle-resolved photoemission spectroscopy (ARPES) on trigonal tellurium consisting of helical chains in the crystal. Through the band-structure mapping in the three-dimensional Brillouin zone, we found a definitive evidence for the band splitting originating from the chiral nature of crystal. A direct comparison of the band dispersion between the ARPES results and the first-principles band-structure calculations suggests the presence of Weyl nodes and tiny spin-polarized hole pockets around the H point. The present result opens a pathway toward studying the interplay among crystal symmetry, band structure, and exotic physical properties in chiral crystals.

Shubnikov–de Haas oscillation of Bi2Te3 topological insulators with cm-scale uniformity

A topological insulating Bi2Te3 single crystal was successfully grown with good uniformity using a home-made resistance-heated floated zone furnace. The temperature-dependent resistance and Hall voltage confirm that the transport is metallic and the overall carriersareholes. The angle and temperature dependence of the quantum Shubnikov–de Haas oscillation period amplitude suggests that the transport comes from the carriers of surface states. The Berry phase, determined from Landau level diagram, also reveals that the transport carriers are Dirac fermions. In contrast with many previous publications, the transport parameters relating to the surface carriers derived from the relationship of the Lifshitz–Kosevich (LK) theory are consistent with angle resolved photoemission spectroscopy results.