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1.
Nanomaterials (Basel) ; 11(11)2021 Oct 31.
Artigo em Inglês | MEDLINE | ID: mdl-34835687

RESUMO

The strain in hybrid van der Waals heterostructures, made of two distinct two-dimensional van der Waals materials, offers an interesting handle on their corresponding electronic band structure. Such strain can be engineered by changing the relative crystallographic orientation between the constitutive monolayers, notably, the angular misorientation, also known as the "twist angle". By combining angle-resolved photoemission spectroscopy with density functional theory calculations, we investigate here the band structure of the WS2/graphene heterobilayer for various twist angles. Despite the relatively weak coupling between WS2 and graphene, we demonstrate that the resulting strain quantitatively affects many electronic features of the WS2 monolayers, including the spin-orbit coupling strength. In particular, we show that the WS2 spin-orbit splitting of the valence band maximum at K can be tuned from 430 to 460 meV. Our findings open perspectives in controlling the band dispersion of van der Waals materials.

2.
Nano Lett ; 21(10): 4415-4422, 2021 May 26.
Artigo em Inglês | MEDLINE | ID: mdl-33978424

RESUMO

Spatially controlling the Fermi level of topological insulators and keeping their electronic states stable are indispensable processes to put this material into practical use for semiconductor spintronics devices. So far, however, such a method has not been established yet. Here we show a novel method for doping a hole into n-type topological insulators Bi2X3 (X= Se, Te) that overcomes the shortcomings of the previous reported methods. The key of this doping is to adsorb H2O on Bi2X3 decorated with a small amount of carbon, and its trigger is the irradiation of a photon with sufficient energy to excite the core electrons of the outermost layer atoms. This method allows controlling the doping amount by the irradiation time and acts as photolithography. Such a tunable doping makes it possible to design the electronic states at the nanometer scale and, thus, paves a promising avenue toward the realization of novel spintronics devices based on topological insulators.

4.
ACS Appl Mater Interfaces ; 12(36): 40525-40531, 2020 Sep 09.
Artigo em Inglês | MEDLINE | ID: mdl-32805799

RESUMO

Photocurrent production in quasi-one-dimensional (1D) transition-metal trichalcogenides, TiS3(001) and ZrS3(001), was examined using polarization-dependent scanning photocurrent microscopy. The photocurrent intensity was the strongest when the excitation source was polarized along the 1D chains with dichroic ratios of 4:1 and 1.2:1 for ZrS3 and TiS3, respectively. This behavior is explained by symmetry selection rules applicable to both valence and conduction band states. Symmetry selection rules are seen to be applicable to the experimental band structure, as is observed in polarization-dependent nanospot angle-resolved photoemission spectroscopy. Based on these band symmetry assignments, it is expected that the dichroic ratios for both materials will be maximized using excitation energies within 1 eV of their band gaps, providing versatile polarization sensitive photodetection across the visible spectrum and into the near-infrared.

5.
Nat Nanotechnol ; 15(10): 861-867, 2020 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-32719494

RESUMO

Multilayer graphene and its stacking order provide both fundamentally intriguing properties and technological engineering applications. Several approaches to control the stacking order have been demonstrated, but a method of precisely controlling the number of layers with desired stacking sequences is still lacking. Here, we propose an approach for controlling the layer thickness and crystallographic stacking sequence of multilayer graphene films at the wafer scale via Cu-Si alloy formation using direct chemical vapour deposition. C atoms are introduced by tuning the ultra-low-limit CH4 concentration to form a SiC layer, reaching one to four graphene layers at the wafer scale after Si sublimation. The crystallographic structure of single-crystalline or uniformly oriented bilayer (AB), trilayer (ABA) and tetralayer (ABCA) graphene are determined via nano-angle-resolved photoemission spectroscopy, which agrees with theoretical calculations, Raman spectroscopy and transport measurements. The present study takes a step towards the layer-controlled growth of graphite and other two-dimensional materials.

6.
J Phys Condens Matter ; 32(29): 29LT01, 2020 Jul 08.
Artigo em Inglês | MEDLINE | ID: mdl-32209749

RESUMO

The band structure of the quasi-one-dimensional transition metal trichalcogenide ZrS3(001) was investigated using nanospot angle resolved photoemission spectroscopy (nanoARPES) and shown to have many similarities with the band structure of TiS3(001). We find that ZrS3, like TiS3, is strongly n-type with the top of the valence band ∼1.9 eV below the Fermi level, at the center of the surface Brillouin zone. The nanoARPES spectra indicate that the top of the valence band of the ZrS3(001) is located at [Formula: see text]. The band structure of both TiS3 and ZrS3 exhibit strong in-plane anisotropy, which results in a larger hole effective mass along the quasi-one-dimensional chains than perpendicular to them.

7.
Nat Commun ; 11(1): 546, 2020 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-31992694

RESUMO

The properties of van der Waals (vdW) materials often vary dramatically with the atomic stacking order between layers, but this order can be difficult to control. Trilayer graphene (TLG) stacks in either a semimetallic ABA or a semiconducting ABC configuration with a gate-tunable band gap, but the latter has only been produced by exfoliation. Here we present a chemical vapor deposition approach to TLG growth that yields greatly enhanced fraction and size of ABC domains. The key insight is that substrate curvature can stabilize ABC domains. Controllable ABC yields ~59% were achieved by tailoring substrate curvature levels. ABC fractions remained high after transfer to device substrates, as confirmed by transport measurements revealing the expected tunable ABC band gap. Substrate topography engineering provides a path to large-scale synthesis of epitaxial ABC-TLG and other vdW materials.

8.
ACS Nano ; 13(9): 10210-10220, 2019 Sep 24.
Artigo em Inglês | MEDLINE | ID: mdl-31442021

RESUMO

For quasi-freestanding 2H-TaS2 in monolayer thickness grown by in situ molecular beam epitaxy on graphene on Ir(111), we find unambiguous evidence for a charge density wave close to a 3 × 3 periodicity. Using scanning tunneling spectroscopy, we determine the magnitude of the partial charge density wave gap. Angle-resolved photoemission spectroscopy, complemented by scanning tunneling spectroscopy for the unoccupied states, makes a tight-binding fit for the band structure of the TaS2 monolayer possible. As hybridization with substrate bands is absent, the fit yields a precise value for the doping of the TaS2 layer. Additional Li doping shifts the charge density wave to a 2 × 2 periodicity. Unexpectedly, the bilayer of TaS2 also displays a disordered 2 × 2 charge density wave. Calculations of the phonon dispersions based on a combination of density-functional theory, density-functional perturbation theory, and many-body perturbation theory enable us to provide phase diagrams for the TaS2 charge density wave as functions of doping, hybridization, and interlayer potentials, and offer insight into how they affect lattice dynamics and stability. Our theoretical considerations are consistent with the experimental work presented and shed light on previous experimental and theoretical investigations of related systems.

9.
Nano Lett ; 19(7): 4641-4650, 2019 Jul 10.
Artigo em Inglês | MEDLINE | ID: mdl-31189314

RESUMO

We clarify that the chemisorption of oxygen atoms at the edges is a key contributor to the frequently observed edge enhancement and spatial non-uniformities of photoluminescence (PL) in WS2 monolayers. Here we have investigated with momentum- and real-space nanoimaging of the chemical and electronic density inhomogeneity of WS2 flakes. Our finding from a large panoply of techniques together with density functional theory calculation confirms that the oxygen chemisorption leads to the electron accumulation at the edges. This facilitates the trion dominance of PL at the edges of WS2 flakes. Our results highlight and unravel the significance of chemisorbed oxygen at the edges in the PL emission and electronic structure of WS2, providing a viable path to enhance the performance of transition-metal-dichalcogenide-based devices.

10.
ACS Nano ; 13(1): 803-811, 2019 Jan 22.
Artigo em Inglês | MEDLINE | ID: mdl-30586504

RESUMO

We explore the electrical characteristics of TiS3 nanowire field-effect transistor (FETs), over the wide temperature range from 3 to 350 K. These nanomaterials have a quasi-one-dimensional (1D) crystal structure and exhibit a gate-controlled metal-insulator transition (MIT) in their transfer curves. Their room-temperature mobility is ∼20-30 cm2/(V s), 2 orders of magnitude smaller than predicted previously, a result that we explain quantitatively in terms of the influence of polar-optical phonon scattering in these materials. In the insulating state (<∼220 K), the transfer curves exhibit unusual mesoscopic fluctuations and a current suppression near zero bias that is common to charge-density wave (CDW) systems. The fluctuations have a nonmonotonic temperature dependence and wash out at a temperature close to that of the bulk MIT, suggesting they may be a feature of quantum interference in the CDW state. Overall, our results demonstrate that quasi-1D TiS3 nanostructures represent a viable candidate for FET realization and that their functionality is influenced by complex phenomena.

11.
Nat Mater ; 17(11): 1048, 2018 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-30262907

RESUMO

The authors unanimously wish to retract this Article due to their concerns about the interpretation of the low-energy electron microscopy (LEEM) and diffraction (LEED) patterns reported in the manuscript. In this study, the authors used spatial and angle-resolved photoemission spectroscopy (ARPES) to characterize graphene monolayers grown on copper foils, and observed regions of graphene adlayers with enhanced graphene/Cu interaction, higher Dirac cone doping level, moiré mini Dirac cones and large lattice expansion. All these properties have been clearly verified and reproduced by photoemission spectroscopy as well as explained by density functional theory. LEEM and LEED characterization were also carried out to confirm the existence of a moiré superlattice and lattice expansion, and the results were included in the main manuscript and Supplementary Information. On further analysis of the LEEM/LEED data, it seems that while the existence of a moiré superlattice can be corroborated, the conclusion of graphene lattice expansion (7%) based on spatially resolved ARPES determinations cannot be confirmed by the LEEM/LEED measurements. The authors realized that these measurements were collected from statistically non-representative areas of the sample. Moreover, the fact that the raw microLEED images bear an asymmetry factor of as much as 5% due to the instrumental aberration makes it impossible to estimate any compression or expansion of the same order. Consequently, their conclusion on the graphene lattice expansion can only be supported by the photoemission data. In view that more complete and reliable structural determinations should be conducted, all authors wish to retract this Article.

12.
ACS Nano ; 12(8): 7571-7582, 2018 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-30004663

RESUMO

We investigate the electronic and vibrational properties of bottom-up synthesized aligned armchair graphene nanoribbons of N = 7 carbon atoms width periodically doped by substitutional boron atoms (B-7AGNRs). Using angle-resolved photoemission spectroscopy and density functional theory calculations, we find that the dopant-derived valence and conduction band states are notably hybridized with electronic states of Au substrate and spread in energy. The interaction with the substrate leaves the bands with pure carbon character rather unperturbed. This results in an identical effective mass of ≈0.2 m0 for the next-highest valence band compared with pristine 7AGNRs. We probe the phonons of B-7AGNRs by ultrahigh-vacuum (UHV) Raman spectroscopy and reveal the existence of characteristic splitting and red shifts in Raman modes due to the presence of substitutional boron atoms. Comparing the Raman spectra for three visible lasers (red, green, and blue), we find that interaction with gold suppresses the Raman signal from B-7AGNRs and the energy of the green laser (2.33 eV) is closer to the resonant E22 transition. The hybridized electronic structure of the B-7AGNR-Au interface is expected to improve electrical characteristics of contacts between graphene nanoribbon and Au. The Raman fingerprint allows the easy identification of B-7AGNRs, which is particularly useful for device fabrication.

13.
Nano Lett ; 18(8): 4664-4668, 2018 08 08.
Artigo em Inglês | MEDLINE | ID: mdl-29991260

RESUMO

Transition-metal dichalcogenides exhibit strong quantum confinement effects, and their electronic structure is strongly dependent on the number of layers. Resolving the thickness-dependent electronic structure is important. While the electronic structure of atomically thin 2H-MoSe2 or 2H-MoS2 have been explored, information on the experimental electronic structure of 2H-MoTe2 is still missing. Here, by using nanospot angle-resolved photoemission spectroscopy (nanoARPES), we reveal the experimental electronic structure of exfoliated 2H-MoTe2 thin flakes with different thickness (three, five, and seven monolayers). Well-separated quantum-well states are clearly observed in thin 2H-MoTe2 flakes at deep valence bands at energies between -3 to -5 eV, while those at the top of the valence band between -1 and -2 eV are much more closely spaced compared with those from 2H-MoSe2 and 2H-MoS2. First-principles calculation shows that the main difference is attributed to the weaker hybridization and smaller energy difference between Mo 4d z2 and Te 5p z orbitals as compared with Se 4p z and S 3p z orbitals. Our work demonstrates the power of nanoARPES in resolving the electronic structure of atomically thin exfoliated flakes.

14.
Adv Mater ; 30(30): e1800754, 2018 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-29893020

RESUMO

2D layered materials have emerged in recent years as a new platform to host novel electronic, optical, or excitonic physics and develop unprecedented nanoelectronic and energy applications. By definition, these materials are strongly anisotropic between the basal plane and cross the plane. The structural and property anisotropies inside their basal plane, however, are much less investigated. Black phosphorus, for example, is a 2D material that has such in-plane anisotropy. Here, a rare chemical form of arsenic, called black-arsenic (b-As), is reported as a cousin of black phosphorus, as an extremely anisotropic layered semiconductor. Systematic characterization of the structural, electronic, thermal, and electrical properties of b-As single crystals is performed, with particular focus on its anisotropies along two in-plane principle axes, armchair (AC) and zigzag (ZZ). The analysis shows that b-As exhibits higher or comparable electronic, thermal, and electric transport anisotropies between the AC and ZZ directions than any other known 2D crystals. Such extreme in-plane anisotropies can potentially implement novel ideas for scientific research and device applications.

15.
Proc Natl Acad Sci U S A ; 115(27): 6928-6933, 2018 07 03.
Artigo em Inglês | MEDLINE | ID: mdl-29915054

RESUMO

The interlayer coupling can be used to engineer the electronic structure of van der Waals heterostructures (superlattices) to obtain properties that are not possible in a single material. So far research in heterostructures has been focused on commensurate superlattices with a long-ranged Moiré period. Incommensurate heterostructures with rotational symmetry but not translational symmetry (in analogy to quasicrystals) are not only rare in nature, but also the interlayer interaction has often been assumed to be negligible due to the lack of phase coherence. Here we report the successful growth of quasicrystalline 30° twisted bilayer graphene (30°-tBLG), which is stabilized by the Pt(111) substrate, and reveal its electronic structure. The 30°-tBLG is confirmed by low energy electron diffraction and the intervalley double-resonance Raman mode at 1383 cm-1 Moreover, the emergence of mirrored Dirac cones inside the Brillouin zone of each graphene layer and a gap opening at the zone boundary suggest that these two graphene layers are coupled via a generalized Umklapp scattering mechanism-that is, scattering of a Dirac cone in one graphene layer by the reciprocal lattice vector of the other graphene layer. Our work highlights the important role of interlayer coupling in incommensurate quasicrystalline superlattices, thereby extending band structure engineering to incommensurate superstructures.

16.
Nat Mater ; 17(5): 450-455, 2018 05.
Artigo em Inglês | MEDLINE | ID: mdl-29632409

RESUMO

Variations of the lattice parameter can significantly change the properties of a material, and, in particular, its electronic behaviour. In the case of graphene, however, variations of the lattice constant with respect to graphite have been limited to less than 2.5% due to its well-established high in-plane stiffness. Here, through systematic electronic and lattice structure studies, we report regions where the lattice constant of graphene monolayers grown on copper by chemical vapour deposition increases up to ~7.5% of its relaxed value. Density functional theory calculations confirm that this expanded phase is energetically metastable and driven by the enhanced interaction between the substrate and the graphene adlayer. We also prove that this phase possesses distinctive chemical and electronic properties. The inherent phase complexity of graphene grown on copper foils revealed in this study may inspire the investigation of possible metastable phases in other seemingly simple heterostructure systems.

17.
Sci Rep ; 7(1): 5145, 2017 07 11.
Artigo em Inglês | MEDLINE | ID: mdl-28698655

RESUMO

ReSe2 and ReS2 are unusual compounds amongst the layered transition metal dichalcogenides as a result of their low symmetry, with a characteristic in-plane anisotropy due to in-plane rhenium 'chains'. They preserve inversion symmetry independent of the number of layers and, in contrast to more well-known transition metal dichalcogenides, bulk and few-monolayer Re-TMD compounds have been proposed to behave as electronically and vibrational decoupled layers. Here, we probe for the first time the electronic band structure of bulk ReSe2 by direct nanoscale angle-resolved photoemission spectroscopy. We find a highly anisotropic in- and out-of-plane electronic structure, with the valence band maxima located away from any particular high-symmetry direction. The effective mass doubles its value perpendicular to the Re chains and the interlayer van der Waals coupling generates significant electronic dispersion normal to the layers. Our density functional theory calculations, including spin-orbit effects, are in excellent agreement with these experimental findings.

18.
Sci Rep ; 7: 46394, 2017 04 12.
Artigo em Inglês | MEDLINE | ID: mdl-28401962

RESUMO

The achievement of the superlubricity regime, with a friction coefficient below 0.01, is the Holy Grail of many tribological applications, with the potential to have a remarkable impact on economic and environmental issues. Based on a combined high-resolution photoemission and soft X-ray absorption study, we report that superlubricity can be realized for engineering applications in bearing steel coated with ultra-smooth tetrahedral amorphous carbon (ta-C) under oleic acid lubrication. The results show that tribochemical reactions promoted by the oil lubrication generate strong structural changes in the carbon hybridization of the ta-C hydrogen-free carbon, with initially high sp3 content. Interestingly, the macroscopic superlow friction regime of moving mechanical assemblies coated with ta-C can be attributed to a few partially oxidized graphene-like sheets, with a thickness of not more than 1 nm, formed at the surface inside the wear scar. The sp2 planar carbon and oxygen-derived species are the hallmark of these mesoscopic surface structures created on top of colliding asperities as a result of the tribochemical reactions induced by the oleic acid lubrication. Atomistic simulations elucidate the tribo-formation of such graphene-like structures, providing the link between the overall atomistic mechanism and the macroscopic experimental observations of green superlubricity in the investigated ta-C/oleic acid tribological systems.

19.
J Phys Condens Matter ; 29(18): 183001, 2017 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-28260698

RESUMO

Electronic structure, which describes the distribution of electronic states in reciprocal space, is one of the most fundamental concepts in condensed matter physics, since it determines the electrical, optical and magnetic behaviours of materials. Graphene has great promise for both fundamental physics and future applications. Chemical vapour deposition (CVD) is currently the dominant technology for its scaled growth on metal foils. The polycrystalline nature of metal foil makes NanoARPES, one energy-momentum dispersion probe with spatial resolution down to a few tens of nanometers, a unique tool to study the intrinsic electronic structure of polycrystalline graphene films. In this topical review, we present the latest NanoARPES studies on graphene grains and films grown on copper foil by CVD. The comprehensive chemical and electronic images probed by NanoARPES provide deep insight about graphene and point out potential ways to functionalize graphene properties. This knowledge may stimulate us to look into the future of this field from both the material synthesis and the instrumental characterisation.

20.
Nat Commun ; 8: 14231, 2017 02 06.
Artigo em Inglês | MEDLINE | ID: mdl-28165445

RESUMO

Material line defects are one-dimensional structures but the search and proof of electron behaviour consistent with the reduced dimension of such defects has been so far unsuccessful. Here we show using angle resolved photoemission spectroscopy that twin-grain boundaries in the layered semiconductor MoSe2 exhibit parabolic metallic bands. The one-dimensional nature is evident from a charge density wave transition, whose periodicity is given by kF/π, consistent with scanning tunnelling microscopy and angle resolved photoemission measurements. Most importantly, we provide evidence for spin- and charge-separation, the hallmark of one-dimensional quantum liquids. Our studies show that the spectral line splits into distinctive spinon and holon excitations whose dispersions exactly follow the energy-momentum dependence calculated by a Hubbard model with suitable finite-range interactions. Our results also imply that quantum wires and junctions can be isolated in line defects of other transition metal dichalcogenides, which may enable quantum transport measurements and devices.


Assuntos
Elétrons , Modelos Teóricos , Espectroscopia Fotoeletrônica , Semicondutores , Microscopia de Tunelamento , Molibdênio/química , Selênio/química
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