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1.
Phys Rev Lett ; 124(3): 036402, 2020 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-32031832

RESUMO

Platinum ditelluride (PtTe_{2}), a type-II Dirac semimetal, remains semimetallic in ultrathin films down to just two triatomic layers (TLs) with a negative gap of -0.36 eV. Further reduction of the film thickness to a single TL induces a Lifshitz electronic transition to a semiconductor with a large positive gap of +0.79 eV. This transition is evidenced by experimental band structure mapping of films prepared by layer-resolved molecular beam epitaxy, and by comparing the data to first-principles calculations using a hybrid functional. The results demonstrate a novel electronic transition at the two-dimensional limit through film thickness control.

2.
Nano Lett ; 20(1): 95-100, 2020 Jan 08.
Artigo em Inglês | MEDLINE | ID: mdl-31752490

RESUMO

Identifying material parameters affecting properties of ferromagnets is key to optimized materials that are better suited for spintronics. Magnetic anisotropy is of particular importance in van der Waals magnets, since it not only influences magnetic and spin transport properties, but also is essential to stabilizing magnetic order in the two-dimensional limit. Here, we report that hole doping effectively modulates the magnetic anisotropy of a van der Waals ferromagnet and explore the physical origin of this effect. Fe3-xGeTe2 nanoflakes show a significant suppression of the magnetic anisotropy with hole doping. Electronic structure measurements and calculations reveal that the chemical potential shift associated with hole doping is responsible for the reduced magnetic anisotropy by decreasing the energy gain from the spin-orbit induced band splitting. Our findings provide an understanding of the intricate connection between electronic structures and magnetic properties in two-dimensional magnets and propose a method to engineer magnetic properties through doping.

3.
Nano Lett ; 19(8): 5634-5639, 2019 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-31329449

RESUMO

We report the creation and manipulation of structural phase boundaries in the single-layer quantum spin Hall insulator 1T'-WSe2 by means of scanning tunneling microscope tip pulses. We observe the formation of one-dimensional interfaces between topologically nontrivial 1T' domains having different rotational orientations, as well as induced interfaces between topologically nontrivial 1T' and topologically trivial 1H phases. Scanning tunneling spectroscopy measurements show that 1T'/1T' interface states are localized at domain boundaries, consistent with theoretically predicted unprotected interface modes that form dispersive bands in and around the energy gap of this quantum spin Hall insulator. We observe a qualitative difference in the experimental spectral line shape between topologically "unprotected" states at 1T'/1T' domain boundaries and protected states at 1T'/1H and 1T'/vacuum boundaries in single-layer WSe2.

4.
Nat Commun ; 10(1): 3382, 2019 Jul 29.
Artigo em Inglês | MEDLINE | ID: mdl-31358753

RESUMO

Chalcogen vacancies are generally considered to be the most common point defects in transition metal dichalcogenide (TMD) semiconductors because of their low formation energy in vacuum and their frequent observation in transmission electron microscopy studies. Consequently, unexpected optical, transport, and catalytic properties in 2D-TMDs have been attributed to in-gap states associated with chalcogen vacancies, even in the absence of direct experimental evidence. Here, we combine low-temperature non-contact atomic force microscopy, scanning tunneling microscopy and spectroscopy, and state-of-the-art ab initio density functional theory and GW calculations to determine both the atomic structure and electronic properties of an abundant chalcogen-site point defect common to MoSe2 and WS2 monolayers grown by molecular beam epitaxy and chemical vapor deposition, respectively. Surprisingly, we observe no in-gap states. Our results strongly suggest that the common chalcogen defects in the described 2D-TMD semiconductors, measured in vacuum environment after gentle annealing, are oxygen substitutional defects, rather than vacancies.

6.
Nature ; 564(7736): 390-394, 2018 12.
Artigo em Inglês | MEDLINE | ID: mdl-30532002

RESUMO

The electric-field-induced quantum phase transition from topological to conventional insulator has been proposed as the basis of a topological field effect transistor1-4. In this scheme, 'on' is the ballistic flow of charge and spin along dissipationless edges of a two-dimensional quantum spin Hall insulator5-9, and 'off' is produced by applying an electric field that converts the exotic insulator to a conventional insulator with no conductive channels. Such a topological transistor is promising for low-energy logic circuits4, which would necessitate electric-field-switched materials with conventional and topological bandgaps much greater than the thermal energy at room temperature, substantially greater than proposed so far6-8. Topological Dirac semimetals are promising systems in which to look for topological field-effect switching, as they lie at the boundary between conventional and topological phases3,10-16. Here we use scanning tunnelling microscopy and spectroscopy and angle-resolved photoelectron spectroscopy to show that mono- and bilayer films of the topological Dirac semimetal3,17 Na3Bi are two-dimensional topological insulators with bulk bandgaps greater than 300 millielectronvolts owing to quantum confinement in the absence of electric field. On application of electric field by doping with potassium or by close approach of the scanning tunnelling microscope tip, the Stark effect completely closes the bandgap and re-opens it as a conventional gap of 90 millielectronvolts. The large bandgaps in both the conventional and quantum spin Hall phases, much greater than the thermal energy at room temperature (25 millielectronvolts), suggest that ultrathin Na3Bi is suitable for room-temperature topological transistor operation.

7.
Sci Rep ; 8(1): 15322, 2018 Oct 17.
Artigo em Inglês | MEDLINE | ID: mdl-30333501

RESUMO

We investigate the electronic structure of BaMnBi2 and BaZnBi2 using angle-resolved photoemission spectroscopy and first-principles calculations. Although they share similar structural properties, we show that their electronic structure exhibit dramatic differences. A strong anisotropic Dirac dispersion is revealed in BaMnBi2 with a decreased asymmetry factor compared with other members of AMnBi2 (A = alkali earth or rare earth elements) family. In addition to the Dirac cones, multiple bands crossing the Fermi energy give rise to a complex Fermi surface topology for BaZnBi2. We further show that the strength of hybridization between Bi-p and Mn-d/Zn-s states is the main driver of the differences in electronic structure for these two related compounds.

8.
Nat Commun ; 9(1): 3401, 2018 08 24.
Artigo em Inglês | MEDLINE | ID: mdl-30143617

RESUMO

Transition metal dichalcogenide materials are unique in the wide variety of structural and electronic phases they exhibit in the two-dimensional limit. Here we show how such polymorphic flexibility can be used to achieve topological states at highly ordered phase boundaries in a new quantum spin Hall insulator (QSHI), 1T'-WSe2. We observe edge states at the crystallographically aligned interface between a quantum spin Hall insulating domain of 1T'-WSe2 and a semiconducting domain of 1H-WSe2 in contiguous single layers. The QSHI nature of single-layer 1T'-WSe2 is verified using angle-resolved photoemission spectroscopy to determine band inversion around a 120 meV energy gap, as well as scanning tunneling spectroscopy to directly image edge-state formation. Using this edge-state geometry we confirm the predicted penetration depth of one-dimensional interface states into the two-dimensional bulk of a QSHI for a well-specified crystallographic direction. These interfaces create opportunities for testing predictions of the microscopic behavior of topologically protected boundary states.

9.
Nano Lett ; 18(6): 3661-3666, 2018 06 13.
Artigo em Inglês | MEDLINE | ID: mdl-29761696

RESUMO

The interaction between a magnetic impurity, such as cerium (Ce) atom, and surrounding electrons has been one of the core problems in understanding many-body interaction in solid and its relation to magnetism. Kondo effect, the formation of a new resonant ground state with quenched magnetic moment, provides a general framework to describe many-body interaction in the presence of magnetic impurity. In this Letter, a combined study of angle-resolved photoemission (ARPES) and dynamic mean-field theory (DMFT) on Ce-intercalated graphene shows that Ce-induced localized states near Fermi energy, EF, hybridized with the graphene π-band, exhibit gradual increase in spectral weight upon decreasing temperature. The observed temperature dependence follows the expectations from the Kondo picture in the weak coupling limit. Our results provide a novel insight how Kondo physics emerges in the sea of two-dimensional Dirac electrons.

10.
Nano Lett ; 18(2): 689-694, 2018 02 14.
Artigo em Inglês | MEDLINE | ID: mdl-29300484

RESUMO

We present the electronic characterization of single-layer 1H-TaSe2 grown by molecular beam epitaxy using a combined angle-resolved photoemission spectroscopy, scanning tunneling microscopy/spectroscopy, and density functional theory calculations. We demonstrate that 3 × 3 charge-density-wave (CDW) order persists despite distinct changes in the low energy electronic structure highlighted by the reduction in the number of bands crossing the Fermi energy and the corresponding modification of Fermi surface topology. Enhanced spin-orbit coupling and lattice distortion in the single-layer play a crucial role in the formation of CDW order. Our findings provide a deeper understanding of the nature of CDW order in the two-dimensional limit.

11.
Nano Lett ; 18(2): 1099-1103, 2018 02 14.
Artigo em Inglês | MEDLINE | ID: mdl-29286670

RESUMO

The monochromatic photoemission from diamondoid monolayers provides a new strategy to create electron sources with low energy dispersion and enables compact electron guns with high brightness and low beam emittance for aberration-free imaging, lithography, and accelerators. However, these potential applications are hindered by degradation of diamondoid monolayers under photon irradiation and electron bombardment. Here, we report a graphene-protected diamondoid monolayer photocathode with 4-fold enhancement of stability compared to the bare diamondoid counterpart. The single-layer graphene overcoating preserves the monochromaticity of the photoelectrons, showing 12.5 meV ful width at half-maximum distribution of kinetic energy. Importantly, the graphene coating effectively suppresses desorption of the diamondoid monolayer, enhancing its thermal stability by at least 100 K. Furthermore, by comparing the decay rate at different photon energies, we identify electron bombardment as the principle decay pathway for diamondoids under graphene protection. This provides a generic approach for stabilizing volatile species on photocathode surfaces, which could greatly improve performance of electron emitters.

12.
Nano Lett ; 17(12): 7339-7344, 2017 12 13.
Artigo em Inglês | MEDLINE | ID: mdl-29111764

RESUMO

The unique electronic band structure of indium nitride InN, part of the industrially significant III-N class of semiconductors, offers charge transport properties with great application potential due to its robust n-type conductivity. Here, we explore the water sensing mechanism of InN thin films. Using angle-resolved photoemission spectroscopy, core level spectroscopy, and theory, we derive the charge carrier density and electrical potential of a two-dimensional electron gas, 2DEG, at the InN surface and monitor its electronic properties upon in situ modulation of adsorbed water. An electric dipole layer formed by water molecules raises the surface potential and accumulates charge in the 2DEG, enhancing surface conductivity. Our intuitive model provides a novel route toward understanding the water sensing mechanism in InN and, more generally, for understanding sensing material systems beyond InN.

13.
Nano Lett ; 17(10): 5914-5918, 2017 10 11.
Artigo em Inglês | MEDLINE | ID: mdl-28906124

RESUMO

The electron band structure of graphene on SrTiO3 substrate has been investigated as a function of temperature. The high-resolution angle-resolved photoemission study reveals that the spectral width at Fermi energy and the Fermi velocity of graphene on SrTiO3 are comparable to those of graphene on a BN substrate. Near the charge neutrality, the energy-momentum dispersion of graphene exhibits a strong deviation from the well-known linearity, which is magnified as temperature decreases. Such modification resembles the characteristics of enhanced electron-electron interaction. Our results not only suggest that SrTiO3 can be a plausible candidate as a substrate material for applications in graphene-based electronics but also provide a possible route toward the realization of a new type of strongly correlated electron phases in the prototypical two-dimensional system via the manipulation of temperature and a proper choice of dielectric substrates.

14.
Nanoscale ; 9(32): 11498-11503, 2017 Aug 17.
Artigo em Inglês | MEDLINE | ID: mdl-28766659

RESUMO

The interaction between graphene and substrates provides a viable route to enhance the functionality of both materials. Depending on the nature of electronic interaction at the interface, the electron band structure of graphene is strongly influenced, allowing us to make use of the intrinsic properties of graphene or to design additional functionalities in graphene. Here, we present an angle-resolved photoemission study on the interaction between graphene and a platinum substrate. The formation of an interface between graphene and platinum leads to a strong deviation in the electronic structure of graphene not only from its freestanding form but also from the behavior observed on typical metals. The combined study on the experimental and theoretical electron band structure unveils the unique electronic properties of graphene on a platinum substrate, which singles out graphene/platinum as a model system investigating graphene on a metallic substrate with strong interaction.

15.
Phys Rev Lett ; 118(14): 146402, 2017 Apr 07.
Artigo em Inglês | MEDLINE | ID: mdl-28430465

RESUMO

Three-dimensional (3D) topological Dirac semimetals (TDSs) are rare but important as a versatile platform for exploring exotic electronic properties and topological phase transitions. A quintessential feature of TDSs is 3D Dirac fermions associated with bulk electronic states near the Fermi level. Using angle-resolved photoemission spectroscopy, we have observed such bulk Dirac cones in epitaxially grown α-Sn films on InSb(111), the first such TDS system realized in an elemental form. First-principles calculations confirm that epitaxial strain is key to the formation of the TDS phase. A phase diagram is established that connects the 3D TDS phase through a singular point of a zero-gap semimetal phase to a topological insulator phase. The nature of the Dirac cone crosses over from 3D to 2D as the film thickness is reduced.

16.
Nat Commun ; 8: 14468, 2017 02 10.
Artigo em Inglês | MEDLINE | ID: mdl-28186084

RESUMO

The observation of replica bands in single-unit-cell FeSe on SrTiO3 (STO)(001) by angle-resolved photoemission spectroscopy (ARPES) has led to the conjecture that the coupling between FeSe electrons and the STO phonons are responsible for the enhancement of Tc over other FeSe-based superconductors. However the recent observation of a similar superconducting gap in single-unit-cell FeSe/STO(110) raised the question of whether a similar mechanism applies. Here we report the ARPES study of the electronic structure of FeSe/STO(110). Similar to the results in FeSe/STO(001), clear replica bands are observed. We also present a comparative study of STO(001) and STO(110) bare surfaces, and observe similar replica bands separated by approximately the same energy, indicating this coupling is a generic feature of the STO surfaces and interfaces. Our findings suggest that the large superconducting gaps observed in FeSe films grown on different STO surface terminations are likely enhanced by a common mechanism.

17.
J Phys Condens Matter ; 28(45): 454001, 2016 11 16.
Artigo em Inglês | MEDLINE | ID: mdl-27617696

RESUMO

Few-layer thick MoSe2 and WSe2 possess non-trivial spin textures with sizable spin splitting due to the inversion symmetry breaking embedded in the crystal structure and strong spin-orbit coupling. We report a spin-resolved photoemission study of MoSe2 and WSe2 thin film samples epitaxially grown on a bilayer graphene substrate. We only found spin polarization in the single- and trilayer samples-not in the bilayer sample-mostly along the out-of-plane direction of the sample surface. The measured spin polarization is found to be strongly dependent on the light polarization as well as the measurement geometry, which reveals intricate coupling between the spin and orbital degrees of freedom in this class of material.

18.
Nano Lett ; 16(8): 4738-45, 2016 08 10.
Artigo em Inglês | MEDLINE | ID: mdl-27357620

RESUMO

Layered transition metal chalcogenides with large spin orbit coupling have recently sparked much interest due to their potential applications for electronic, optoelectronic, spintronics, and valleytronics. However, most current understanding of the electronic structure near band valleys in momentum space is based on either theoretical investigations or optical measurements, leaving the detailed band structure elusive. For example, the exact position of the conduction band valley of bulk MoS2 remains controversial. Here, using angle-resolved photoemission spectroscopy with submicron spatial resolution (micro-ARPES), we systematically imaged the conduction/valence band structure evolution across representative chalcogenides MoS2, WS2, and WSe2, as well as the thickness dependent electronic structure from bulk to the monolayer limit. These results establish a solid basis to understand the underlying valley physics of these materials, and also provide a link between chalcogenide electronic band structure and their physical properties for potential valleytronics applications.

19.
Nano Lett ; 16(4): 2485-91, 2016 Apr 13.
Artigo em Inglês | MEDLINE | ID: mdl-26974978

RESUMO

High quality WSe2 films have been grown on bilayer graphene (BLG) with layer-by-layer control of thickness using molecular beam epitaxy. The combination of angle-resolved photoemission, scanning tunneling microscopy/spectroscopy, and optical absorption measurements reveal the atomic and electronic structures evolution and optical response of WSe2/BLG. We observe that a bilayer of WSe2 is a direct bandgap semiconductor, when integrated in a BLG-based heterostructure, thus shifting the direct-indirect band gap crossover to trilayer WSe2. In the monolayer limit, WSe2 shows a spin-splitting of 475 meV in the valence band at the K point, the largest value observed among all the MX2 (M = Mo, W; X = S, Se) materials. The exciton binding energy of monolayer-WSe2/BLG is found to be 0.21 eV, a value that is orders of magnitude larger than that of conventional three-dimensional semiconductors, yet small as compared to other two-dimensional transition metal dichalcogennides (TMDCs) semiconductors. Finally, our finding regarding the overall modification of the electronic structure by an alkali metal surface electron doping opens a route to further control the electronic properties of TMDCs.

20.
J Synchrotron Radiat ; 22(3): 776-80, 2015 May.
Artigo em Inglês | MEDLINE | ID: mdl-25931096

RESUMO

Soft X-ray angle-resolved photoemission has been performed for metallic V2O3. By combining a microfocus beam (40 µm × 65 µm) and micro-positioning techniques with a long-working-distance microscope, it has been possible to observe band dispersions from tiny cleavage surfaces with a typical size of several tens of µm. The photoemission spectra show a clear position dependence, reflecting the morphology of the cleaved sample surface. By selecting high-quality flat regions on the sample surface, it has been possible to perform band mapping using both photon-energy and polar-angle dependences, opening the door to three-dimensional angle-resolved photoemission spectroscopy for typical three-dimensional correlated materials where large cleavage planes are rarely obtained.

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