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The Weyl semimetals represent a distinct category of topological materials wherein the low-energy excitations appear as the long-sought Weyl Fermions. Exotic transport and optical properties are expected because of the chiral anomaly and linear energy-momentum dispersion. While three-dimensional Weyl semimetals have been successfully realized, the quest for their two-dimensional (2D) counterparts is ongoing. Here, we report the realization of 2D Weyl Fermions in monolayer PtTe1.75, which has strong spin-orbit coupling and lacks inversion symmetry, by combined angle-resolved photoemission spectroscopy, scanning tunneling microscopy, second harmonic generation, X-ray photoelectron spectroscopy measurements, and first-principles calculations. The giant Rashba splitting and band inversion lead to the emergence of three pairs of critical Weyl cones. Moreover, monolayer PtTe1.75 exhibits excellent chemical stability in ambient conditions, which is critical for future device applications. The discovery of 2D Weyl Fermions in monolayer PtTe1.75 opens up new possibilities for designing and fabricating novel spintronic devices.
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Dirac materials, which feature Dirac cones in the reciprocal space, have been one of the hottest topics in condensed matter physics in the past decade. To date, 2D and 3D Dirac Fermions have been extensively studied, while their 1D counterparts are rare. Recently, Si nanoribbons (SiNRs), which are composed of alternating pentagonal Si rings, have attracted intensive attention. However, the electronic structure and topological properties of SiNRs are still elusive. Here, by angle-resolved photoemission spectroscopy, scanning tunneling microscopy/spectroscopy measurements, first-principles calculations, and tight-binding model analysis, we demonstrate the existence of 1D Dirac Fermions in SiNRs. Our theoretical analysis shows that the Dirac cones derive from the armchairlike Si chain in the center of the nanoribbon and can be described by the Su-Schrieffer-Heeger model. These results establish SiNRs as a platform for studying the novel physical properties in 1D Dirac materials.
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The destructive interference of wavefunctions in a kagome lattice can give rise to topological flat bands (TFBs) with a highly degenerate state of electrons. Recently, TFBs have been observed in several kagome metals, including Fe3Sn2, FeSn, CoSn, and YMn6Sn6. Nonetheless, kagome materials that are both exfoliable and semiconducting are lacking, which seriously hinders their device applications. Herein, we show that Nb3Cl8, which hosts a breathing kagome lattice, is gapped out because of the absence of inversion symmetry, while the TFBs survive because of the protection of the mirror reflection symmetry. By angle-resolved photoemission spectroscopy measurements and first-principles calculations, we directly observe the TFBs and a moderate band gap in Nb3Cl8. By mechanical exfoliation, we successfully obtain monolayer Nb3Cl8, which is stable under ambient conditions. In addition, our calculations show that monolayer Nb3Cl8 has a magnetic ground state, thus providing opportunities to study the interplay among geometry, topology, and magnetism.
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The spin polarization in nonmagnetic materials is conventionally attributed to the outcome of spin-orbit coupling when the global inversion symmetry is broken. The recently discovered hidden spin polarization indicates that a specific atomic site asymmetry could also induce measurable spin polarization, leading to a paradigm shift in research on centrosymmetric crystals for potential spintronic applications. Here, combining spin- and angle-resolved photoemission spectroscopy and theoretical calculations, we report distinct spin-momentum-layer locking phenomena in a centrosymmetric, layered material, BiOI. The measured spin is highly polarized along the Brillouin zone boundary, while the same effect almost vanishes around the zone center due to its nonsymmorphic crystal structure. Our work demonstrates the existence of momentum-dependent hidden spin polarization and uncovers the microscopic mechanism of spin, momentum, and layer locking to each other, thus shedding light on the design metrics for future spintronic materials.
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The charge density wave (CDW) in ZrTe_{3} is quenched in samples with a small amount of Te isoelectronically substituted by Se. Using angle-resolved photoemission spectroscopy we observe subtle changes in the electronic band dispersions and Fermi surfaces upon Se substitution. The scattering rates are substantially increased, in particular for the large three-dimensional Fermi surface sheet. The quasi-one-dimensional band is unaffected by the substitution and still shows a gap at low temperature, which starts to open from room temperature. Long-range order is, however, absent in the electronic states as in the periodic lattice distortion. The competition between superconductivity and the CDW is thus linked to the suppression of long-range order of the CDW.
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We demonstrate that the excitonic insulator ground state of Ta_{2}NiSe_{5} can be electrically controlled by electropositive surface adsorbates. Our studies utilizing angle-resolved photoemission spectroscopy reveal intriguing wave-vector-dependent deformations of the characteristic flattop valence band of this material upon potassium adsorption. The observed band deformation indicates a reduction of the single-particle band gap due to the Stark effect near the surface. The present study provides the foundation for the electrical tuning of the many-body quantum states in excitonic insulators.
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Atomic scale engineering of two-dimensional materials could create devices with rich physical and chemical properties. External periodic potentials can enable the manipulation of the electronic band structures of materials. A prototypical system is (3×3)-silicene/Ag(111), which has substrate-induced periodic modulations. Recent angle-resolved photoemission spectroscopy measurements revealed six Dirac cone pairs at the Brillouin zone boundary of Ag(111), but their origin remains unclear [Proc. Natl. Acad. Sci. USA 113, 14656 (2016)]. We used linear dichroism angle-resolved photoemission spectroscopy, the tight-binding model, and first-principles calculations to reveal that these Dirac cones mainly derive from the original cones at the K (K^{'}) points of free-standing silicene. The Dirac cones of free-standing silicene are split by external periodic potentials that originate from the substrate-overlayer interaction. Our results not only confirm the origin of the Dirac cones in the (3×3)-silicene/Ag(111) system, but also provide a powerful route to manipulate the electronic structures of two-dimensional materials.
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Two-dimensional (2D) materials have attracted great attention and spurred rapid development in both fundamental research and device applications. The search for exotic physical properties, such as magnetic and topological order, in 2D materials could enable the realization of novel quantum devices and is therefore at the forefront of materials science. Here, we report the discovery of twofold degenerate Weyl nodal lines in a 2D ferromagnetic material, a single-layer gadolinium-silver compound, based on combined angle-resolved photoemission spectroscopy measurements and theoretical calculations. These Weyl nodal lines are symmetry protected and thus robust against external perturbations. The coexistence of magnetic and topological order in a 2D material is likely to inform ongoing efforts study the rich physics in 2D topological ferromagnets.
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We report the electronic structure of CuTe with a high charge density wave (CDW) transition temperature T_{c}=335 K by angle-resolved photoemission spectroscopy. An anisotropic charge density wave gap with a maximum value of 190 meV is observed in the quasi-one-dimensional band formed by Te p_{x} orbitals. The CDW gap can be filled by increasing the temperature or electron doping through in situ potassium deposition. Combining the experimental results with calculated electron scattering susceptibility and phonon dispersion, we suggest that both Fermi surface nesting and electron-phonon coupling play important roles in the emergence of the CDW.
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We performed annealing and angle resolved photoemission spectroscopy studies on electron-doped cuprate Pr_{1-x}LaCe_{x}CuO_{4-δ} (PLCCO). It is found that the optimal annealing condition is dependent on the Ce content x. The electron number (n) is estimated from the experimentally obtained Fermi surface volume for x=0.10, 0.15 and 0.18 samples. It clearly shows a significant and annealing dependent deviation from the nominal x. In addition, we observe that the pseudo-gap at hot spots is also closely correlated with n; the pseudogap gradually closes as n increases. We established a new phase diagram of PLCCO as a function of n. Different from the x-based one, the new phase diagram shows similar antiferromagnetic and superconducting phases to those of hole doped ones. Our results raise a possibility for absence of disparity between the phase diagrams of electron- and hole-doped cuprates.
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Single-layer transition-metal dichalcogenides (TMDs) receive significant attention due to their intriguing physical properties for both fundamental research and potential applications in electronics, optoelectronics, spintronics, catalysis, and so on. Here, we demonstrate the epitaxial growth of high-quality single-crystal, monolayer platinum diselenide (PtSe2), a new member of the layered TMDs family, by a single step of direct selenization of a Pt(111) substrate. A combination of atomic-resolution experimental characterizations and first-principle theoretic calculations reveals the atomic structure of the monolayer PtSe2/Pt(111). Angle-resolved photoemission spectroscopy measurements confirm for the first time the semiconducting electronic structure of monolayer PtSe2 (in contrast to its semimetallic bulk counterpart). The photocatalytic activity of monolayer PtSe2 film is evaluated by a methylene-blue photodegradation experiment, demonstrating its practical application as a promising photocatalyst. Moreover, circular polarization calculations predict that monolayer PtSe2 has also potential applications in valleytronics.
Assuntos
Processos Fotoquímicos , Platina/química , Compostos de Selênio/química , SemicondutoresRESUMO
The surface state of a Z(2) topological insulator connects with the conduction and valence band continua of the bulk, thereby bridging the band gap of the volume. We investigate this connection of the surface and bulk electronic structure for Sb(2)Te(3)(0001) by photoemission experiments and calculations. Upon crossing the topmost valence band the topological surface state (TSS) maintains a coherent spectral signature, a two-dimensional character, and a linear dispersion relation. Surface-bulk coupling manifests itself in the spectra through (i) a characteristic kink in the TSS dispersion as it crosses the topmost valence band and (ii) the appearance of hybridization gaps between the TSS and bulk-derived surface resonance states at higher binding energies. The findings provide a natural explanation for the unexpectedly weak surface-bulk mixing indicated by recent transport experiments on Sb(2)Te(3).
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Recently, unconventional antiferromagnets that enable the spin splitting (SS) of electronic states have been theoretically proposed and experimentally realized, where the magnetic sublattices containing moments pointing at different directions are connected by a novel set of symmetries. Such SS is substantial, k-dependent, and independent of the spin-orbit coupling (SOC) strength, making these magnets promising materials for antiferromagnetic spintronics. Here, combined with angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT) calculations, a systematic study on CrSb, a metallic spin-split antiferromagnet candidate with Néel temperature TN = 703 K, is conducted. The data reveal the electronic structure of CrSb along both out-of-plane and in-plane momentum directions, rendering an anisotropic k-dependent SS that agrees well with the calculational results. The magnitude of such SS reaches up to at least 0.8 eV at non-high-symmetry momentum points, which is significantly higher than the largest known SOC-induced SS. This compound expands the choice of materials in the field of antiferromagnetic spintronics and is likely to stimulate subsequent investigations of high-efficiency spintronic devices that are functional at room temperature.
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The possibility that a pairing boson might act as the 'glue' to bind electrons into a Cooper pair in superconductors with a high critical temperature (T(c)) is being actively pursued in condensed-matter physics. Gweon et al. claim that there is a large and unusual oxygen-isotope effect on the electronic structure, indicating that phonons have a special importance in high-temperature superconductors. However, we are unable to detect this unusual oxygen-isotope effect in new data collected under almost identical material and experimental conditions. Our findings point towards a more conventional influence of phonons in these materials.
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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.
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We performed angle-resolved photoemission (ARPES) experiments with circularly polarized light and first-principles density functional calculation with spin-orbit coupling to study surface states of a topological insulator Bi2Se3. We observed circular dichroism (CD) as large as 30% in the ARPES data with upper and lower Dirac cones showing opposite signs in CD. The observed CD is attributed to the existence of local orbital-angular momentum (OAM). First-principles calculation shows that OAM in the surface states is significant and is locked to the electron momentum in the opposite direction to the spin, forming chiral OAM states. Our finding opens a new possibility for strong light-induced spin-polarized current in surface states. We also provide a proof for local OAM origin of the CD in ARPES.
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In this review, an attempt has been made to compare the electronic structures of various 5d iridates (iridium oxides), with an effort to note the common features and differences. Both experimental studies, especially angle-resolved photoemission spectroscopy (ARPES) results, and first-principles band structure calculations have been discussed. This brings to focus the fact that the electronic structures and magnetic properties of the high-Z 5d transition iridates depend on the intricate interplay of strong electron correlation, strong (relativistic) spin-orbit coupling, lattice distortion, and the dimensionality of the system. For example, in the thin film limit, SrIrO3 exhibits a metal-insulator transition that corresponds to the dimensionality crossover, with the band structure resembling that of bulk Sr2IrO4.
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Emergent phenomena such as unconventional superconductivity, Mott-like insulators, and the peculiar quantum Hall effect in graphene-based heterostructures are proposed to stem from the superlattice-induced renormalization of (moiré) Dirac fermions at the graphene Brillouin zone corners. Understanding the corresponding band structure commonly demands photoemission spectroscopy with both sub-meV resolution and large-momentum coverage, beyond the capability of the current state-of-the-art. Here the realization of moiré Dirac cones around the Brillouin zone center in monolayer In2 Se3 /bilayer graphene heterostructure is reported. The renormalization is evidenced by reduced Fermi velocity (≈23%) of the moiré Dirac cones and the reshaped Dirac point at the Γ point where they intersect. While there have been many theoretical predictions and much indirect experimental evidence, the findings here are the first direct observation of Fermi velocity reduction of the moiré Dirac cones. These features suggest strong In2 Se3 /graphene interlayer coupling, which is comparable with that in twisted bilayer graphene. The strategy expands the choice of materials in the heterostructure design and stimulates subsequent broad investigations of emergent physics at the sub-meV energy scale.
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Lateral heterojunctions of atomically precise graphene nanoribbons (GNRs) hold promise for applications in nanotechnology, yet their charge transport and most of the spectroscopic properties have not been investigated. Here, we synthesize a monolayer of multiple aligned heterojunctions consisting of quasi-metallic and wide-bandgap GNRs, and report characterization by scanning tunneling microscopy, angle-resolved photoemission, Raman spectroscopy, and charge transport. Comprehensive transport measurements as a function of bias and gate voltages, channel length, and temperature reveal that charge transport is dictated by tunneling through the potential barriers formed by wide-bandgap GNR segments. The current-voltage characteristics are in agreement with calculations of tunneling conductance through asymmetric barriers. We fabricate a GNR heterojunctions based sensor and demonstrate greatly improved sensitivity to adsorbates compared to graphene based sensors. This is achieved via modulation of the GNR heterojunction tunneling barriers by adsorbates.
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The electronic transport properties of conventional three-dimensional metals are successfully described by Fermi-liquid theory. But when the dimensionality of such a system is reduced to one, the Fermi-liquid state becomes unstable to Coulomb interactions, and the conduction electrons should instead behave according to Tomonaga-Luttinger-liquid (TLL) theory. Such a state reveals itself through interaction-dependent anomalous exponents in the correlation functions, density of states and momentum distribution of the electrons. Metallic single-walled carbon nanotubes (SWNTs) are considered to be ideal one-dimensional systems for realizing TLL states. Indeed, the results of transport measurements on metal-SWNT and SWNT-SWNT junctions have been attributed to the effects of tunnelling into or between TLLs, although there remains some ambiguity in these interpretations. Direct observations of the electronic states in SWNTs are therefore needed to resolve these uncertainties. Here we report angle-integrated photoemission measurements of SWNTs. Our results reveal an oscillation in the pi-electron density of states owing to one-dimensional van Hove singularities, confirming the one-dimensional nature of the valence band. The spectral function and intensities at the Fermi level both exhibit power-law behaviour (with almost identical exponents) in good agreement with theoretical predictions for the TLL state in SWNTs.