Angle-resolved Photoemission Spectroscopy Measurements Research Articles

Experimental observation of node-line-like surface states in LaBi

In a Dirac nodal line semimetal, the bulk conduction and valence bands touch at extended lines in the Brillouin zone. To date, most of the theoretically predicted and experimentally discovered nodal lines derive from the bulk bands of two- and three-dimensional materials. Here, based on combined angle-resolved photoemission spectroscopy measurements and first-principles calculations, we report the discovery of node-line-like surface states on the (001) surface of LaBi. These bands derive from the topological surface states of LaBi and bridge the band gap opened by spin-orbit coupling and band inversion. Our first-principles calculations reveal that these "nodal lines" have a tiny gap, which is beyond typical experimental resolution. These results may provide important information to understand the extraordinary physical properties of LaBi, such as the extremely large magnetoresistance and resistivity plateau.

Electronic band structure of Two-Dimensional WS2 /Graphene van der Waals Heterostructures

Combining single-layer two-dimensional semiconducting transition metal dichalcogenides (TMDs) with graphene layer in van der Waals heterostructures offers an intriguing means of controlling the electronic properties through these heterostructures. Here, we report the electronic and structural properties of transferred single layer WS2 on epitaxial graphene using micro-Raman spectroscopy, angle-resolved photoemission spectroscopy measurements (ARPES) and Density Functional Theory (DFT) calculations. The results show good electronic properties as well as well-defined band arising from the strong splitting of the single layer WS2 valence band at K points, with a maximum splitting of 0.44 eV. By comparing our DFT results with local and hybrid functionals, we find the top valence band of the experimental heterostructure is close to the calculations for suspended single layer WS2. . Our results provide an important reference for future studies of electronic properties of WS2 and its applications in valleytronic devices.

Two-dimensional electronic transport and surface electron accumulation in MoS2

Because the surface-to-volume ratio of quasi-two-dimensional materials is extremely high, understanding their surface characteristics is crucial for practically controlling their intrinsic properties and fabricating p-type and n-type layered semiconductors. Van der Waals crystals are expected to have an inert surface because of the absence of dangling bonds. However, here we show that the surface of high-quality synthesized molybdenum disulfide (MoS2) is a major n-doping source. The surface electron concentration of MoS2 is nearly four orders of magnitude higher than that of its inner bulk. Substantial thickness-dependent conductivity in MoS2 nanoflakes was observed. The transfer length method suggested the current transport in MoS2 following a two-dimensional behavior rather than the conventional three-dimensional mode. Scanning tunneling microscopy and angle-resolved photoemission spectroscopy measurements confirmed the presence of surface electron accumulation in this layered material. Notably, the in situ-cleaved surface exhibited a nearly intrinsic state without electron accumulation.

Converting topological insulators into topological metals within the tetradymite family

We report the electronic band structures and concomitant Fermi surfaces for a family of exfoliable tetradymite compounds with the formula $T_2$$Ch_2$$Pn$, obtained as a modification to the well-known topological insulator binaries Bi$_2$(Se,Te)$_3$ by replacing one chalcogen ($Ch$) with a pnictogen ($Pn$) and Bi with the tetravalent transition metals $T$ $=$ Ti, Zr, or Hf. This imbalances the electron count and results in layered metals characterized by relatively high carrier mobilities and bulk two-dimensional Fermi surfaces whose topography is well-described by first principles calculations. Intriguingly, slab electronic structure calculations predict Dirac-like surface states. In contrast to Bi$_2$Se$_3$, where the surface Dirac bands are at the $\Gamma-$point, for (Zr,Hf)$_2$Te$_2$(P,As) there are Dirac cones of strong topological character around both the $\bar {\Gamma}$- and $\bar {M}$-points which are above and below the Fermi energy, respectively. For Ti$_2$Te$_2$P the surface state is predicted to exist only around the $\bar {M}$-point. In agreement with these predictions, the surface states that are located below the Fermi energy are observed by angle resolved photoemission spectroscopy measurements, revealing that they coexist with the bulk metallic state. Thus, this family of materials provides a foundation upon which to develop novel phenomena that exploit both the bulk and surface states (e.g., topological superconductivity).

Superconducting pairing of topological surface states in bismuth selenide films on niobium.

A topological insulator film coupled to a simple isotropic s-wave superconductor substrate can foster helical pairing of the Dirac fermions associated with the topological surface states. Experimental realization of such a system is exceedingly difficult, however using a novel "flip-chip" technique, we have prepared single-crystalline Bi2Se3 films with predetermined thicknesses in terms of quintuple layers (QLs) on top of Nb substrates fresh from in situ cleavage. Our angle-resolved photoemission spectroscopy (ARPES) measurements of the film surface disclose superconducting gaps and coherence peaks of similar magnitude for both the topological surface states and bulk states. The ARPES spectral map as a function of temperature and film thickness up to 10 QLs reveals key characteristics relevant to the mechanism of coupling between the topological surface states and the superconducting Nb substrate; the effective coupling length is found to be much larger than the decay length of the topological surface states.

Topological Electride Y2C.

Two-dimensional (2D) electrides are layered ionic crystals in which anionic electrons are confined in the interlayer space. Here, we report a discovery of nontrivial [Formula: see text] topology in the electronic structures of 2D electride Y2C. Based on first-principles calculations, we found a topological [Formula: see text] invariant of (1; 111) for the bulk band and topologically protected surface states in the surfaces of Y2C, signifying its nontrivial electronic topology. We suggest a spin-resolved angle-resolved photoemission spectroscopy (ARPES) measurement to detect the unique helical spin texture of the spin-polarized topological surface state, which will provide characteristic evidence for the nontrivial electronic topology of Y2C. Furthermore, the coexistence of 2D surface electride states and topological surface state enables us to explain the outstanding discrepancy between the recent ARPES experiments and theoretical calculations. Our findings establish a preliminary link between the electride in chemistry and the band topology in condensed-matter physics, which are expected to inspire further interdisciplinary research between these fields.

Modification of Vapor Phase Concentrations in MoS2 Growth Using a NiO Foam Barrier.

Single-layer molybdenum disulfide (MoS2) has attracted significant attention due to its electronic and physical properties, with much effort invested toward obtaining large-area high-quality monolayer MoS2 films. In this work, we demonstrate a reactive-barrier-based approach to achieve growth of highly homogeneous single-layer MoS2 on sapphire by the use of a nickel oxide foam barrier during chemical vapor deposition. Due to the reactivity of the NiO barrier with MoO3, the concentration of precursors reaching the substrate and thus nucleation density is effectively reduced, allowing grain sizes of up to 170 μm and continuous monolayers on the centimeter length scale being obtained. The quality of the monolayer is further revealed by angle-resolved photoemission spectroscopy measurement by observation of a very well resolved electronic band structure and spin-orbit splitting of the bands at room temperature with only two major domain orientations, indicating the successful growth of a highly crystalline and well-oriented MoS2 monolayer.

Gapped electronic structure of epitaxial stanene on InSb(111)

Stanene (single-layer grey tin), with an electronic structure akin to that of graphene but exhibiting a much larger spin-orbit gap, offers a promising platform for room-temperature electronics based on the quantum spin Hall (QSH) effect. This material has received much theoretical attention, but a suitable substrate for stanene growth that results in an overall gapped electronic structure has been elusive; a sizable gap is necessary for room-temperature applications. Here, we report a study of stanene epitaxially grown on the (111)B-face of indium antimonide (InSb). Angle-resolved photoemission spectroscopy (ARPES) measurements reveal a gap of 0.44 eV, in agreement with our first-principles calculations. The results indicate that stanene on InSb(111) is a strong contender for electronic QSH applications.

The Key Ingredients of the Electronic Structure of FeSe

FeSe is a fascinating superconducting material at the frontier of research in condensed matter physics. Here, we provide an overview of the current understanding of the electronic structure of FeSe, focusing in particular on its low-energy electronic structure as determined from angle-resolved photoemission spectroscopy, quantum oscillations, and magnetotransport measurements of single-crystal samples. We discuss the unique place of FeSe among iron-based superconductors, as it is a multiband system exhibiting strong orbitally dependent electronic correlations and unusually small Fermi surfaces and is prone to different electronic instabilities. We pay particular attention to the evolution of the electronic structure that accompanies the tetragonal-orthorhombic structural distortion of the lattice around 90 K, which stabilizes a unique nematic electronic state. Finally, we discuss how the multiband multiorbital nematic electronic structure impacts our understanding of the superconductivity, and show that the tunability of the nematic state with chemical and physical pressure helps to disentangle the role of different competing interactions relevant for enhancing superconductivity.

Multiple Types of Topological Fermions in Transition Metal Silicides.

Exotic massless fermionic excitations with nonzero Berry flux, other than the Dirac and Weyl fermions, could exist in condensed matter systems under the protection of crystalline symmetries, such as spin-1 excitations with threefold degeneracy and spin-3/2 Rarita-Schwinger-Weyl fermions. Herein, by using the abinitio density functional theory, we show that these unconventional quasiparticles coexist with type-I and type-II Weyl fermions in a family of transition metal silicides, including CoSi, RhSi, RhGe, and CoGe, when spin-orbit coupling is considered. Their nontrivial topology results in a series of extensive Fermi arcs connecting projections of these bulk excitations on the side surface, which is confirmed by (001) surface electronic spectra of CoSi. In addition, these stable arc states exist within a wide energy window around the Fermi level, which makes them readily accessible in angle-resolved photoemission spectroscopy measurements.

Effects of film thickness and magnetism on the electronic structure of MnO films

We investigate the influence of film thickness and magnetism on the electronic structure of a strongly correlated prototypical system, MnO(001) films epitaxially grown on Ag(001), using angle-resolved photoemission spectroscopy (ARPES) and x-ray photoelectron spectroscopy (XPS) techniques. XPS measurements have confirmed the MnO stoichiometry as well as the layer-by-layer growth mode of the films, while the ARPES measurements have confirmed the high structural quality of the films by the observation of clear band dispersions devoid of any sample charging effects. For lower coverage films, finite-size effects/reduced correlation effects are observed, while from 3 ML coverages, bulklike band structures are formed. Detailed band mapping along $\overline{\mathrm{\ensuremath{\Gamma}}}\text{\ensuremath{-}}\overline{X}$ and $\overline{\mathrm{\ensuremath{\Gamma}}}\text{\ensuremath{-}}\overline{M}$ directions reveal a relative dispersion between Mn-derived ${e}_{g}$ and ${t}_{2g}$ states up to 1.2 eV, in contrast to previous ARPES results where maximum relative dispersions of $\ifmmode\pm\else\textpm\fi{}0.1$ eV were reported, while our results excellently match with the theoretically predicted dispersions. By comparing with theoretical results we show the hybridization between O $2p$ with the Mn ${e}_{g}$ states giving rise to the observed dispersions resulting from the highly dispersive nature of the O $2p$ bands. Furthermore, we show that during the paramagnetic (PM) to antiferromagnetic (AFM) transition, the valence band gets narrower with an enhancement of the $^{5}e_{g}$ peak intensity, along with the widening of the energy gap by 200 meV. Theoretically, Terakura et al. had predicted the possibility of a similar outcome due to the decrease of the effective $dd$ hopping between the oppositely magnetized cations during the PM to AFM-II transition because of the $dd\ensuremath{\sigma}$ type interaction, yet the experimental verification was absent in the literature. We believe that the exact same mechanism as predicted by Terakura et al. is responsible for the changes seen in the electronic structure during magnetic phase transition and argue that a similar trend can be seen for the prototype materials such as CoO and NiO.

Experimental realization of two-dimensional Dirac nodal line fermions in monolayer Cu2Si

Topological nodal line semimetals, a novel quantum state of materials, possess topologically nontrivial valence and conduction bands that touch at a line near the Fermi level. The exotic band structure can lead to various novel properties, such as long-range Coulomb interaction and flat Landau levels. Recently, topological nodal lines have been observed in several bulk materials, such as PtSn4, ZrSiS, TlTaSe2 and PbTaSe2. However, in two-dimensional materials, experimental research on nodal line fermions is still lacking. Here, we report the discovery of two-dimensional Dirac nodal line fermions in monolayer Cu2Si based on combined theoretical calculations and angle-resolved photoemission spectroscopy measurements. The Dirac nodal lines in Cu2Si form two concentric loops centred around the Γ point and are protected by mirror reflection symmetry. Our results establish Cu2Si as a platform to study the novel physical properties in two-dimensional Dirac materials and provide opportunities to realize high-speed low-dissipation devices.

Electronic anisotropies revealed by detwinned angle-resolved photo-emission spectroscopy measurements of FeSe

We report high resolution angle-resolved photo-emission spectroscopy (ARPES) measurements of detwinned FeSe single crystals. The application of a mechanical strain is used to promote the volume fraction of one of the orthorhombic domains in the sample, which we estimate to be detwinned. While the full structure of the electron pockets consisting of two crossed ellipses may be observed in the tetragonal phase at temperatures above 90 K, we find that remarkably, only one peanut-shaped electron pocket oriented along the longer a axis contributes to the ARPES measurement at low temperatures in the nematic phase, with the expected pocket along b being not observed. Thus the low temperature Fermi surface of FeSe as experimentally determined by ARPES consists of one elliptical hole pocket and one orthogonally-oriented peanut-shaped electron pocket. Our measurements clarify the long-standing controversies over the interpretation of ARPES measurements of FeSe.

High-Quality FeTe1−xSex Monolayer Films on SrTiO3(001) Substrates Grown by Molecular Beam Epitaxy**Supported by the Ministry of Science and Technology of China under Grant Nos 2015CB921000, 2016YFA0401000, 2015CB921301 and 2016YFA0300300, and the National Natural Science Foundation of China under Grant Nos 11274381, 11574371, 11274362, 1190020, 11334012 and 11674371.

We report the growth process of FeTe1−xSex () monolayer films on SrTiO3 (STO) substrates through molecular beam epitaxy and discuss the possible ways to improve the film quality. By exploring the parameters of substrate treatment, growth control and post growth annealing, we successfully obtain a series of FeTe1−xSex monolayer films. In the whole growth process, we find the significance of the temperature control through surface roughness monitored by the reflection high-energy electron diffraction and scanning tunneling microscopy. We obtain the best quality of FeSe monolayer films with the STO substrate treated at T = 900–950°C before growth, the FeSe deposited at T = 310°C during growth and annealed at T = 380°C after growth. For FeTe1−xSex (), both the growth temperature and annealing temperature decrease to T = 260°C. According to the angle-resolved photoemission spectroscopy measurements, the superconductivity of the FeTe1−xSex film is robust and insensitive to Se concentration. All the above are instructive for further investigations of the superconductivity in FeTe1−xSex films.

Cascade of Magnetic-Field-Induced Lifshitz Transitions in the Ferromagnetic Kondo Lattice Material YbNi_{4}P_{2}.

A ferromagnetic quantum critical point is thought not to exist in two- and three-dimensional metallic systems yet is realized in the Kondo lattice compound YbNi_{4}(P,As)_{2}, possibly due to its one-dimensionality. It is crucial to investigate the dimensionality of the Fermi surface of YbNi_{4}P_{2} experimentally, but common probes such as angle-resolved photoemission spectroscopy and quantum oscillation measurements are lacking. Here, we study the magnetic-field dependence of transport and thermodynamic properties of YbNi_{4}P_{2}. The Kondo effect is continuously suppressed, and additionally we identify nine Lifshitz transitions between 0.4 and 18T. We analyze the transport coefficients in detail and identify the type of Lifshitz transitions as neck or void type to gain information on the Fermi surface of YbNi_{4}P_{2}. The large number of Lifshitz transitions observed within this small energy window is unprecedented and results from the particular flat renormalized band structure with strong 4f-electron character shaped by the Kondo lattice effect.

Lorentz-violating type-II Dirac fermions in transition metal dichalcogenide PtTe2

Topological semimetals have recently attracted extensive research interests as host materials to condensed matter physics counterparts of Dirac and Weyl fermions originally proposed in high energy physics. Although Lorentz invariance is required in high energy physics, it is not necessarily obeyed in condensed matter physics, and thus Lorentz-violating type-II Weyl/Dirac fermions could be realized in topological semimetals. The recent realization of type-II Weyl fermions raises the question whether their spin-degenerate counterpart—type-II Dirac fermions—can be experimentally realized too. Here, we report the experimental evidence of type-II Dirac fermions in bulk stoichiometric PtTe2 single crystal. Angle-resolved photoemission spectroscopy measurements and first-principles calculations reveal a pair of strongly tilted Dirac cones along the Γ-A direction, confirming PtTe2 as a type-II Dirac semimetal. Our results provide opportunities for investigating novel quantum phenomena (e.g., anisotropic magneto-transport) and topological phase transition.

Proximity-effect-induced Superconducting Gap in Topological Surface States \u2013 A Point Contact Spectroscopy Study of NbSe2/Bi2Se3 Superconductor-Topological Insulator Heterostructures

Proximity-effect-induced superconductivity was studied in epitaxial topological insulator Bi2Se3 thin films grown on superconducting NbSe2 single crystals. A point contact spectroscopy (PCS) method was used at low temperatures down to 40 mK. An induced superconducting gap in Bi2Se3 was observed in the spectra, which decreased with increasing Bi2Se3 layer thickness, consistent with the proximity effect in the bulk states of Bi2Se3 induced by NbSe2. At very low temperatures, an extra point contact feature which may correspond to a second energy gap appeared in the spectrum. For a 16 quintuple layer Bi2Se3 on NbSe2 sample, the bulk state gap value near the top surface is ~159 μeV, while the second gap value is ~120 μeV at 40 mK. The second gap value decreased with increasing Bi2Se3 layer thickness, but the ratio between the second gap and the bulk state gap remained about the same for different Bi2Se3 thicknesses. It is plausible that this is due to superconductivity in Bi2Se3 topological surface states induced through the bulk states. The two induced gaps in the PCS measurement are consistent with the three-dimensional bulk state and the two-dimensional surface state superconducting gaps observed in the angle-resolved photoemission spectroscopy (ARPES) measurement.

Possible spin excitation structure in monolayer FeSe grown on SrTiO3

Based on recent high-resolution angle-resolved photoemission spectroscopy measurement in monolayer FeSe grown on SrTiO$_{3}$, we constructed a tight-binding model and proposed a superconducting (SC) pairing function which can well fit the observed band structure and SC gap anisotropy. Then we investigated the spin excitation spectra in order to determine the possible sign structure of the SC order parameter. We found that a resonance-like spin excitation may occur if the SC order parameter changes sign along the Fermi surfaces. However, this resonance is located at different locations in momentum space compared to other FeSe-based superconductors, suggesting that the Fermi surface shape and pairing symmetry in monolayer FeSe grown on SrTiO$_{3}$ may be different from other FeSe-based superconductors.

Electronic structure of RSb ( R=Y , Ce, Gd, Dy, Ho, Tm, Lu) studied by angle-resolved photoemission spectroscopy

We use high resolution angle-resolved photoemission spectroscopy (ARPES) and electronic structure calculations to study the electronic properties of rare-earth monoantimonides RSb (R = Y, Ce, Gd, Dy, Ho, Tm, Lu). The experimentally measured Fermi surface (FS) of RSb consists of at least two concentric hole pockets at the $\Gamma$ point and two intersecting electron pockets at the $X$ point. These data agree relatively well with the electronic structure calculations. Detailed photon energy dependence measurements using both synchrotron and laser ARPES systems indicate that there is at least one Fermi surface sheet with strong three-dimensionality centered at the $\Gamma$ point. Due to the "lanthanide contraction", the unit cell of different rare-earth monoantimonides shrinks when changing rare-earth ion from CeSb to LuSb. This results in the differences in the chemical potentials in these compounds, which is demonstrated by both ARPES measurements and electronic structure calculations. Interestingly, in CeSb, the intersecting electron pockets at the $X$ point seem to be touching the valence bands, forming a four-fold degenerate Dirac-like feature. On the other hand, the remaining rare-earth monoantimonides show significant gaps between the upper and lower bands at the $X$ point. Furthermore, similar to the previously reported results of LaBi, a Dirac-like structure was observed at the $\Gamma$ point in YSb, CeSb, and GdSb, compounds showing relatively high magnetoresistance. This Dirac-like structure may contribute to the unusually large magnetoresistance in these compounds.

Tunable quasiparticle band gap in few-layer GaSe/graphene van der Waals heterostructures

Two-dimensional (2D) materials have recently been the focus of extensive research. By following a similar trend as graphene, other 2D materials including transition metal dichalcogenides (MX2) and metal mono-chalcogenides (MX) show great potential for ultrathin nanoelectronic and optoelectronic devices. Despite the weak nature of interlayer forces in semiconducting MX materials, their electronic properties are highly dependent on the number of layers. Using scanning tunneling microscopy and spectroscopy (STM/STS), we demonstrate the tunability of the quasiparticle energy gap of few layered gallium selenide (GaSe) directly grown on a bilayer graphene substrate by molecular beam epitaxy (MBE). Our results show that the band gap is about 3.50 +/-0.05 eV for single-tetralayer (1TL), 3.00 +/-0.05 eV for bi-tetralayer (2TL) and 2.30 +/-0.05 eV for tri-tetralayer (3TL). This band gap evolution of GaSe, in particularly the shift of the valence band with respect to the Fermi level, was confirmed by angle-resolved photoemission spectroscopy (ARPES) measurements and our theoretical calculations. Moreover, we observed a charge transfer in GaSe/graphene van der Waals (vdW) heterostructure using ARPES. These findings demonstrate the high impact on the GaSe electronic band structure and electronic properties that can be obtained by the control of 2D materials layer thickness and the graphene induced doping.