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Showing papers on "Scanning tunneling spectroscopy published in 2018"


Journal ArticleDOI
19 Oct 2018-Science
TL;DR: A sharp zero-bias peak inside a vortex core that does not split when moving away from the vortex center is observed, consistent with the tunneling to a nearly pure MBS, separated from nontopological bound states.
Abstract: The search for Majorana bound states (MBSs) has been fueled by the prospect of using their non-Abelian statistics for robust quantum computation. Two-dimensional superconducting topological materials have been predicted to host MBSs as zero-energy modes in vortex cores. By using scanning tunneling spectroscopy on the superconducting Dirac surface state of the iron-based superconductor FeTe0.55Se0.45, we observed a sharp zero-bias peak inside a vortex core that does not split when moving away from the vortex center. The evolution of the peak under varying magnetic field, temperature, and tunneling barrier is consistent with the tunneling to a nearly pure MBS, separated from nontopological bound states. This observation offers a potential platform for realizing and manipulating MBSs at a relatively high temperature.

650 citations


Journal ArticleDOI
TL;DR: A flexible strategy based on atomically precise graphene nanoribbons to design robust nanomaterials exhibiting the valence electronic structures described by the SSH Hamiltonian is presented and controlled periodic coupling of topological boundary states are demonstrated to create quasi-one-dimensional trivial and non-trivial electronic quantum phases.
Abstract: Here we present a flexible strategy to realize robust nanomaterials exhibiting valence electronic structures whose fundamental physics is described by the SSH-Hamiltonian. These solid-state materials are realized using atomically precise graphene nanoribbons (GNR). We demonstrate the controlled periodic coupling of topological boundary states at junctions of armchair GNRs of different widths to create quasi-1D trivial and non-trivial electronic quantum phases. Their topological class is experimentally determined by drawing upon the bulk-boundary correspondence and measuring the presence (non-trivial) or absence (trivial) of localized end states by scanning tunneling spectroscopy (STS). The strategy we propose has the potential to tune the band width of the topological electronic bands close to the energy scale of proximity induced spin-orbit coupling or superconductivity, and may allow the realization of Kitaev like Hamiltonians and Majorana type end states.

285 citations


Journal ArticleDOI
TL;DR: In this paper, it was shown that a zero-bias conductance peak (ZBCP) exists ubiquitously in the cores of free vortices in the defect free regions of (Li0.84Fe0.16)OHFeSe, which has a superconducting transition temperature of 42 K.
Abstract: The Majorana fermion, which is its own anti-particle and obeys non-abelian statistics, plays a critical role in topological quantum computing. It can be realized as a bound state at zero energy, called a Majorana zero mode (MZM), in the vortex core of a topological superconductor, or at the ends of a nanowire when both superconductivity and strong spin orbital coupling are present. A MZM can be detected as a zero-bias conductance peak (ZBCP) in tunneling spectroscopy. However, in practice, clean and robust MZMs have not been realized in the vortices of a superconductor, due to contamination from impurity states or other closely-packed Caroli-de Gennes-Matricon (CdGM) states, which hampers further manipulations of Majorana fermions. Here using scanning tunneling spectroscopy, we show that a ZBCP well separated from the other discrete CdGM states exists ubiquitously in the cores of free vortices in the defect free regions of (Li0.84Fe0.16)OHFeSe, which has a superconducting transition temperature of 42 K. Moreover, a Dirac-cone-type surface state is observed by angle-resolved photoemission spectroscopy, and its topological nature is confirmed by band calculations. The observed ZBCP can be naturally attributed to a MZM arising from this chiral topological surface states of a bulk superconductor. (Li0.84Fe0.16)OHFeSe thus provides an ideal platform for studying MZMs and topological quantum computing.

123 citations


Journal ArticleDOI
TL;DR: A unified approach to the synthesis of the series of higher acenes up to previously unreported undecacene has been developed through the on‐surface dehydrogenation of partially saturated precursors.
Abstract: A unified approach to the synthesis of the series of higher acenes up to previously unreported undecacene has been developed through the on-surface dehydrogenation of partially saturated precursors. These molecules could be converted into the parent acenes by both atomic manipulation with the tip of a scanning tunneling and atomic force microscope (STM/AFM) as well as by on-surface annealing. The structure of the generated acenes has been visualized by high-resolution non-contact AFM imaging and the evolution of the transport gap with the increase of the number of fused benzene rings has been determined on the basis of scanning tunneling spectroscopy (STS) measurements.

114 citations


Journal ArticleDOI
TL;DR: In this article, the authors combine low-temperature noncontact atomic force microscopy (nc-AFM), STS, and state-of-the-art ab initio density functional theory (DFT) and GW calculations to determine both the structure and electronic properties of the most abundant individual chalcogen-site defects common to 2D-TMDs.
Abstract: Chalcogen vacancies are considered to be the most abundant point defects in two-dimensional (2D) transition-metal dichalcogenide (TMD) semiconductors, and predicted to result in deep in-gap states (IGS). As a result, important features in the optical response of 2D-TMDs have typically been attributed to chalcogen vacancies, with indirect support from Transmission Electron Microscopy (TEM) and Scanning Tunneling Microscopy (STM) images. However, TEM imaging measurements do not provide direct access to the electronic structure of individual defects; and while Scanning Tunneling Spectroscopy (STS) is a direct probe of local electronic structure, the interpretation of the chemical nature of atomically-resolved STM images of point defects in 2D-TMDs can be ambiguous. As a result, the assignment of point defects as vacancies or substitutional atoms of different kinds in 2D-TMDs, and their influence on their electronic properties, has been inconsistent and lacks consensus. Here, we combine low-temperature non-contact atomic force microscopy (nc-AFM), STS, and state-of-the-art ab initio density functional theory (DFT) and GW calculations to determine both the structure and electronic properties of the most abundant individual chalcogen-site defects common to 2D-TMDs. Surprisingly, we observe no IGS for any of the chalcogen defects probed. Our results and analysis strongly suggest that the common chalcogen defects in our 2D-TMDs, prepared and measured in standard environments, are substitutional oxygen rather than vacancies.

106 citations


Journal ArticleDOI
TL;DR: In this article, the authors reported the growth of monolayer VSe2 by molecular beam epitaxy (MBE) method, which revealed that the as-grown monolayers VSe 2 has magnetic characteristic peaks in its electronic density of states and a lower work-function at its edges.
Abstract: Recent experimental breakthroughs open up new opportunities for magnetism in few-atomic-layer two-dimensional (2D) materials, which makes fabrication of new magnetic 2D materials a fascinating issue. Here, we report the growth of monolayer VSe2 by molecular beam epitaxy (MBE) method. Electronic properties measurements by scanning tunneling spectroscopy (STS) method revealed that the as-grown monolayer VSe2 has magnetic characteristic peaks in its electronic density of states and a lower work-function at its edges. Moreover, air exposure experiments show air-stability of the monolayer VSe2. This high-quality monolayer VSe2, a very air-inert 2D material with magnetism and low edge work function, is promising for applications in developing next-generation low power-consumption, high efficiency spintronic devices and new electrocatalysts.

105 citations


Journal ArticleDOI
TL;DR: A two-dimensional (2D) heterobilayer system consisting of MoS2 on WSe2, deposited on epitaxial graphene, is studied by scanning tunneling microscopy and spectroscopy at temperatures of 5 and 80 K, and a moiré pattern is observed.
Abstract: A two-dimensional (2D) heterobilayer system consisting of MoS2 on WSe2, deposited on epitaxial graphene, is studied by scanning tunneling microscopy and spectroscopy at temperatures of 5 and 80 K. A moire pattern is observed, arising from lattice mismatch of 3.7% between the MoS2 and WSe2. Significant energy shifts are observed in tunneling spectra observed at the maxima of the moire corrugation, as compared with spectra obtained at corrugation minima, consistent with prior work. Furthermore, at the minima of the moire corrugation, sharp peaks in the spectra at energies near the band edges are observed for spectra acquired at 5 K. The peaks correspond to discrete states that are confined within the moire unit cells. Conductance mapping is employed to reveal the detailed structure of the wave functions of the states. For measurements at 80 K, the sharp peaks in the spectra are absent, and conductance maps of the band edges reveal little structure.

105 citations


Journal ArticleDOI
09 May 2018-ACS Nano
TL;DR: The results suggest that the phosphorene on Au(111) could be a promising candidate, not only for fundamental research but also for nanoelectronics and optoelectronic applications.
Abstract: Exploring stable two-dimensional materials with appropriate band gaps and high carrier mobility is highly desirable due to the potential applications in optoelectronic devices. Here, the electronic structures of phosphorene on a Au(111) substrate are investigated by scanning tunneling spectroscopy, angle-resolved photoemission spectroscopy (ARPES), and density functional theory (DFT) calculations. The substrate-induced phosphorene superstructure gives a superlattice potential, leading to a strong band folding effect of the sp band of Au(111) on the band structure. The band gap could be clearly identified in the ARPES results after examining the folded sp band. The value of the energy gap (∼1.1 eV) and the high charge carrier mobility comparable to that of black phosphorus, which is engineered by the tensile strain, are revealed by the combination of ARPES results and DFT calculations. Furthermore, the phosphorene layer on the Au(111) surface displays high surface inertness, leading to the absence of multi...

82 citations


Journal ArticleDOI
TL;DR: This review of the recent efforts in predicting and understanding the optoelectronic properties of oxides using ab initio theoretical methods discusses the performance of recently developed dielectric-dependent hybrid functionals, providing a comparison against the results of many-body GW calculations.
Abstract: Understanding the electronic structure of metal oxide semiconductors is crucial to their numerous technological applications, such as photoelectrochemical water splitting and solar cells. The needed experimental and theoretical knowledge goes beyond that of pristine bulk crystals, and must include the effects of surfaces and interfaces, as well as those due to the presence of intrinsic defects (e.g. oxygen vacancies), or dopants for band engineering. In this review, we present an account of the recent efforts in predicting and understanding the optoelectronic properties of oxides using ab initio theoretical methods. In particular, we discuss the performance of recently developed dielectric-dependent hybrid functionals, providing a comparison against the results of many-body GW calculations, including G 0 W 0 as well as more refined approaches, such as quasiparticle self-consistent GW. We summarize results in the recent literature for the band gap, the band level alignment at surfaces, and optical transition energies in defective oxides, including wide gap oxide semiconductors and transition metal oxides. Correlated transition metal oxides are also discussed. For each method, we describe successes and drawbacks, emphasizing the challenges faced by the development of improved theoretical approaches. The theoretical section is preceded by a critical overview of the main experimental techniques needed to characterize the optoelectronic properties of semiconductors, including absorption and reflection spectroscopy, photoemission, and scanning tunneling spectroscopy (STS).

82 citations


Journal ArticleDOI
TL;DR: In this paper, the growth of bilayer PdSe2 on a graphene-SiC(0001) substrate by molecular beam epitaxy (MBE) was reported, and a bandgap of 1.15 ± 0.07 eV was revealed by scanning tunneling spectroscopy (STS).
Abstract: Two-dimensional (2D) materials have received significant attention due to their unique physical properties and potential applications in electronics and optoelectronics. Recent studies have demonstrated that exfoliated PdSe2, a layered transition metal dichalcogenide (TMD), exhibits ambipolar field-effect transistor (FET) behavior with notable performance and good air stability, and thus serves as an emerging candidate for 2D electronics. Here, we report the growth of bilayer PdSe2 on a graphene-SiC(0001) substrate by molecular beam epitaxy (MBE). A bandgap of 1.15 ± 0.07 eV was revealed by scanning tunneling spectroscopy (STS). Moreover, a bandgap shift of 0.2 eV was observed in PdSe2 layers grown on monolayer graphene as compared to those grown on bilayer graphene. The realization of nanoscale electronic junctions with atomically sharp boundaries in 2D PdSe2 implies the possibility of tuning its electronic or optoelectronic properties. In addition, on top of the PdSe2 bilayers, PdSe2 nanoribbons and stacks of nanoribbons with a fixed orientation have been fabricated. The bottom-up fabrication of low-dimensional PdSe2 structures is expected to enable substantial exploration of its potential applications.

79 citations


Journal ArticleDOI
TL;DR: Ugeda et al. as mentioned in this paper observed edge states at the crystallographically aligned interface between a single layer quantum spin Hall insulator 1T′-WSe2 and a semiconductor 1H − WSe2 in contiguous single layers and confirmed the predicted penetration depth of one-dimensional interface states into the two-dimensional bulk of a QSHI.
Abstract: 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. Transition metal dichalcogenides may host exotic topological phases in the two-dimensional limit, but detailed atomic properties have rarely been explored. Here, Ugeda et al. observe edge-states at the interface between a single layer quantum spin Hall insulator 1T′-WSe2 and a semiconductor 1H-WSe2.

Journal ArticleDOI
TL;DR: It is found that Td-phase S-doped MoTe2 (MoTe2−xSx, x ∼ 0.2) is a two-band s-wave bulk superconductor, where the superconducting behavior can be explained by the s+− pairing model.
Abstract: Topological Weyl semimetals (TWSs) with pairs of Weyl points and topologically protected Fermi arc states have broadened the classification of topological phases and provide superior platform for study of topological superconductivity Here we report the nontrivial superconductivity and topological features of sulfur-doped Td -phase MoTe2 with enhanced Tc compared with type-II TWS MoTe2 It is found that Td -phase S-doped MoTe2 (MoTe2-x S x , x ∼ 02) is a two-band s-wave bulk superconductor (∼013 meV and 026 meV), where the superconducting behavior can be explained by the s+- pairing model Further, measurements of the quasi-particle interference (QPI) patterns and a comparison with band-structure calculations reveal the existence of Fermi arcs in MoTe2-x S x More interestingly, a relatively large superconducting gap (∼17 meV) is detected by scanning tunneling spectroscopy on the sample surface, showing a hint of topological nontrivial superconductivity based on the pairing of Fermi arc surface states Our work demonstrates that the Td -phase MoTe2-x S x is not only a promising topological superconductor candidate but also a unique material for study of s+- superconductivity

Journal ArticleDOI
TL;DR: In this paper, the authors find a giant renormalization to the free-standing quasiparticle band gap in the presence of metallic substrates, in agreement with recent scanning tunneling spectroscopy and photoluminescence experiments.
Abstract: Monolayer ${\mathrm{MoS}}_{2}$ has emerged as an interesting material for nanoelectronic and optoelectronic devices. The effect of substrate screening and defects on the electronic structure of ${\mathrm{MoS}}_{2}$ are important considerations in the design of such devices. We find a giant renormalization to the free-standing quasiparticle band gap in the presence of metallic substrates, in agreement with recent scanning tunneling spectroscopy and photoluminescence experiments. Our sulfur vacancy defect calculations using the density functional theory plus GW formalism, reveal two charge transition levels (CTLs) in the pristine band gap of ${\mathrm{MoS}}_{2}$. The $(0/\ensuremath{-}1)$ CTL is significantly renormalized with the choice of substrate, with respect to the pristine valence band maximum (VBM). The $(+1/0)$ level, on the other hand, is pinned 100 meV above the pristine VBM for the different substrates. This opens up a pathway to effectively engineer defect charge transition levels in two-dimensional materials through the choice of substrate.

Journal ArticleDOI
TL;DR: Song et al. as mentioned in this paper used the quasiparticle interference technique with scanning tunneling spectroscopy to suppress the bulk conductance in a single-layer 1T-WTe2 topological insulator.
Abstract: The two-dimensional topological insulators host a full gap in the bulk band, induced by spin–orbit coupling (SOC) effect, together with the topologically protected gapless edge states. However, it is usually challenging to suppress the bulk conductance and thus to realize the quantum spin Hall (QSH) effect. In this study, we find a mechanism to effectively suppress the bulk conductance. By using the quasiparticle interference technique with scanning tunneling spectroscopy, we demonstrate that the QSH candidate single-layer 1T’-WTe2 has a semimetal bulk band structure with no full SOC-induced gap. Surprisingly, in this two-dimensional system, we find the electron–electron interactions open a Coulomb gap which is always pinned at the Fermi energy (EF). The opening of the Coulomb gap can efficiently diminish the bulk state at the EF and supports the observation of the quantized conduction of topological edge states. The conductance from bulk bands in a topological insulator usually blurs effects arising from edge states. Here, Song et al. report a Coulomb gap opened by electron–electron interactions, which effectively suppress the bulk conductance and promote observation of topological edge states in the single-layer 1T’-WTe2.

Journal ArticleDOI
TL;DR: It is observed that the hybridization leads to the formation of symmetric and antisymmetric combinations of YSR states, which depend on the shape of the underlying monomer orbitals and the orientation of the dimer with respect to the Pb lattice.
Abstract: Magnetic adsorbates on superconductors induce local bound states within the superconducting gap. These Yu-Shiba-Rusinov (YSR) states decay slowly away from the impurity compared to atomic orbitals, even in 3D bulk crystals. Here, we use scanning tunneling spectroscopy to investigate their hybridization between two nearby magnetic Mn adatoms on a superconducting Pb(001) surface. We observe that the hybridization leads to the formation of symmetric and antisymmetric combinations of YSR states. We investigate how the structure of the dimer wave functions and the energy splitting depend on the shape of the underlying monomer orbitals and the orientation of the dimer with respect to the Pb lattice.

Journal ArticleDOI
TL;DR: This study successfully intercalate potassium into the van der Waals gap of type II Weyl semimetal WTe2 and discovers the superconducting state in K xWTe2 through both electrical transport and scanning tunneling spectroscopy measurements, indicating that the K-intercalated W Te2 may be a promising candidate to explore the topological superconductor.
Abstract: To realize a topological superconductor is one of the most attracting topics because of its great potential in quantum computation In this study, we successfully intercalate potassium (K) into the van der Waals gap of type II Weyl semimetal WTe2 and discover the superconducting state in KxWTe2 through both electrical transport and scanning tunneling spectroscopy measurements The superconductivity exhibits an evident anisotropic behavior Moreover, we also uncover the coexistence of superconductivity and the positive magnetoresistance state Structural analysis substantiates the negligible lattice expansion induced by the intercalation, therefore suggesting K-intercalated WTe2 still hosts the topological nontrivial state These results indicate that the K-intercalated WTe2 may be a promising candidate to explore the topological superconductor

Journal ArticleDOI
08 Mar 2018
TL;DR: In this article, the authors report the observation of metallic edges in atomically thin transition metal dichalcogenides (WSe2) monolayers grown by chemical vapor deposition on epitaxial graphene and demonstrate that the formation of metallic substoichiometric tungsten oxide (WO2.7) is responsible for the high conductivity measured along the edges.
Abstract: Transition metal dichalcogenides are a unique class of layered two-dimensional (2D) crystals with extensive promising applications. Tuning the electronic properties of low-dimensional materials is vital for engineering new functionalities. Surface oxidation is of particular interest because it is a relatively simple method of functionalization. By means of scanning probe microscopy and x-ray photoelectron spectroscopy, we report the observation of metallic edges in atomically thin WSe2 monolayers grown by chemical vapor deposition on epitaxial graphene. Scanning tunneling microscopy shows structural details of WSe2 edges and scanning tunneling spectroscopy reveals the metallic nature of the oxidized edges. Photoemission demonstrates that the formation of metallic sub-stoichiometric tungsten oxide (WO2.7) is responsible for the high conductivity measured along the edges. Ab initio calculations validate the susceptibility of WSe2 nanoribbon edges to oxidation. The zigzag terminated edge exhibits metallic behavior prior the air-exposure and remains metallic after oxidation. Comprehending and exploiting this property opens a new opportunity for application in advanced electronic devices.

Journal ArticleDOI
TL;DR: This method overcomes the limitation of previous on-surface syntheses of –C≡C– incorporated systems, which require the precursors containing alkyne group; it therefore allows for a more flexible design and fabrication of molecular architectures with tailored properties.
Abstract: The carbon-carbon triple bond (-C≡C-) is an elementary constituent for the construction of conjugated molecular wires and carbon allotropes such as carbyne and graphyne. Here we describe a general approach to in situ synthesize -C≡C- bond on Cu(111) surface via homo-coupling of the trichloromethyl groups, enabling the fabrication of individual and arrays of poly(p-phenylene ethynylene) molecular wires. Scanning tunneling spectroscopy reveals a delocalized electronic state extending along these molecular wires, whose structure is unraveled by atomically resolved images of scanning tunneling microscopy and noncontact atomic force microscopy. Combined with density functional theory calculations, we identify the intermediates formed in the sequential dechlorination process, including surface-bound benzyl, carbene, and carbyne radicals. Our method overcomes the limitation of previous on-surface syntheses of -C≡C- incorporated systems, which require the precursors containing alkyne group; it therefore allows for a more flexible design and fabrication of molecular architectures with tailored properties.

Journal ArticleDOI
TL;DR: It is demonstrated that interface engineering by an atomically thin oxide layer is crucial for driving the hybrid system into a topologically nontrivial state as confirmed by theoretical calculations of the topological invariant, the Chern number.
Abstract: Topological superconductors are predicted to harbor exotic boundary states - Majorana zero-energy modes - whose non-Abelian braiding statistics present a new paradigm for the realization of topological quantum computing. Using low-temperature scanning tunneling spectroscopy (STS), we here report on the direct real-space visualization of chiral Majorana edge states in a monolayer topological superconductor, a prototypical magnet-superconductor hybrid system comprised of nano-scale Fe islands of monoatomic height on a Re(0001)-O(2$\times$1) surface. In particular, we demonstrate that interface engineering by an atomically thin oxide layer is crucial for driving the hybrid system into a topologically non-trivial state as confirmed by theoretical calculations of the topological invariant, the Chern number.

Journal ArticleDOI
TL;DR: The results suggest that the ultrathin ALD Al2O3 produced in optimal conditions may provide a low-cost alternative gate dielectric for CMOS and demonstrate the critical importance in controlling the IL to achieving high-performance ultrath in MIM structures.
Abstract: Dielectric properties of ultrathin Al2O3 (1.1-4.4 nm) in metal-insulator-metal (M-I-M) Al/Al2O3/Al trilayers fabricated in situ using an integrated sputtering and atomic layer deposition (ALD) system were investigated. An M-I interfacial layer (IL) formed during the pre-ALD sample transfer even under high vacuum has a profound effect on the dielectric properties of the Al2O3 with a significantly reduced dielectric constant (er) of 0.5-3.3 as compared to the bulk er ∼ 9.2. Moreover, the observed soft-type electric breakdown suggests defects in both the M-I interface and the Al2O3 film. By controlling the pre-ALD exposure to reduce the IL to a negligible level, a high er up to 8.9 was obtained on the ALD Al2O3 films with thicknesses from 3.3 to 4.4 nm, corresponding to an effective oxide thickness (EOT) of ∼1.4-1.9 nm, respectively, which are comparable to the EOTs found in high-K dielectrics like HfO2 at 3-4 nm in thickness and further suggest that the ultrathin ALD Al2O3 produced in optimal conditions may provide a low-cost alternative gate dielectric for CMOS. While er decreases at a smaller Al2O3 thickness, the hard-type dielectric breakdown at 32 MV/cm and in situ scanning tunneling spectroscopy revealed band gap ∼2.63 eV comparable to that of an epitaxial Al2O3 film. This suggests that the IL is unlikely a dominant reason for the reduced er at the Al2O3 thickness of 1.1-2.2 nm but rather a consequence of the electron tunneling as confirmed in the transport measurement. This result demonstrates the critical importance in controlling the IL to achieving high-performance ultrathin dielectric in MIM structures.

Journal ArticleDOI
TL;DR: In this paper, a direct observation of ambipolar self-doping in hybrid lead-iodide perovskites has been reported through scanning tunneling spectroscopy (STS) and, thereby, density of states (DOS).
Abstract: In this work, direct observation of ambipolar self-doping in hybrid lead-iodide perovskites has been reported through scanning tunneling spectroscopy (STS) and, thereby, density of states (DOS). Self-doping phenomenon in CH3NH3PbI3 (MAPbI3) and CH(NH2)2PbI3 (FAPbI3) through precursor stoichiometry has led to an alteration in the Fermi energy, and hence a change in the type of electronic conductivity, without affecting the inherent band gap of the materials. From STS and the respective DOS spectra, the band energies of the perovskites with respect to the Fermi energy for a range of precursor ratios have been estimated. The “direct” measurement of band edges with respect to Fermi energy inferred a gradual change in the electronic conductivity from p-type to n-type as both the perovskites were reacted from PbI2-deficient to PbI2-rich precursors. The results have been correlated with point defects generated due to the growth environment (stoichiometry of precursors) of perovskites, providing a new dimension t...

Journal ArticleDOI
TL;DR: Re6Se8Cl2 is the first member of a new family of 2D semiconductors whose structure is built from superatomic building blocks instead of simply atoms; such structures will expand the conceptual design space for 2D materials research.
Abstract: Structural complexity is of fundamental interest in materials science because it often results in unique physical properties and functions. Founded on this idea, the field of solid state chemistry has a long history and continues to be highly active, with new compounds discovered daily. By contrast, the area of two-dimensional (2D) materials is young, but its expansion, although rapid, is limited by a severe lack of structural diversity and complexity. Here, we report a novel 2D semiconductor with a hierarchical structure composed of covalently linked Re6Se8 clusters. The material, a 2D structural analogue of the Chevrel phase, is prepared via mechanical exfoliation of the van der Waals solid Re6Se8Cl2. Using scanning tunneling spectroscopy, photoluminescence and ultraviolet photoelectron spectroscopy, and first-principles calculations, we determine the electronic bandgap (1.58 eV), optical bandgap (indirect, 1.48 eV), and exciton binding energy (100 meV) of the material. The latter is consistent with the...

Journal ArticleDOI
TL;DR: This work combined scanning tunneling microscopy and locally resolved magnetic stray field measurements on the ferromagnetic semimetal EuB_{6}, which exhibits a complexferromagnetic order and a colossal magnetoresistance effect to show evidence for magnetic clusters also in finite magnetic fields.
Abstract: We combined scanning tunneling microscopy and locally resolved magnetic stray field measurements on the ferromagnetic semimetal EuB_{6}, which exhibits a complex ferromagnetic order and a colossal magnetoresistance effect. In a zero magnetic field, scanning tunneling spectroscopy visualizes the existence of local inhomogeneities in the electronic density of states, which we interpret as the localization of charge carriers due to the formation of magnetic polarons. Micro-Hall magnetometry measurements of the total stray field emanating from the end of a rectangular-shaped platelike sample reveals evidence for magnetic clusters also in finite magnetic fields. In contrast, the signal detected below the faces of the magnetized sample measures a local stray field indicating the formation of pronounced magnetic inhomogeneities consistent with large clusters of percolated magnetic polarons.

Journal ArticleDOI
TL;DR: In this paper, the authors experimentally and theoretically study artificially enhanced spin-orbit coupling in graphene via random decoration with dilute Bi_2Te_3 nanoparticles, and the results highlight a pathway to spintronics and quantum information applications in graphene-based quantum spin Hall platforms.
Abstract: Realization of the quantum spin Hall effect in graphene devices has remained an outstanding challenge dating back to the inception of the field of topological insulators. Graphene’s exceptionally weak spin-orbit coupling—stemming from carbon’s low mass—poses the primary obstacle. We experimentally and theoretically study artificially enhanced spin-orbit coupling in graphene via random decoration with dilute Bi_2Te_3 nanoparticles. Multiterminal resistance measurements suggest the presence of helical edge states characteristic of a quantum spin Hall phase; the magnetic field and temperature dependence of the resistance peaks, x-ray photoelectron spectra, scanning tunneling spectroscopy, and first-principles calculations further support this scenario. These observations highlight a pathway to spintronics and quantum information applications in graphene-based quantum spin Hall platforms.

Journal ArticleDOI
TL;DR: The work suggests a new route to synthesize 1D semimetallic transition metal chalcogenide nanowires, which could serve as ultrasmall conducting building blocks and enable band engineering in future 1D-2D heterostructure devices.
Abstract: Controllable synthesizing of one-dimensional–two-dimensional (1D–2D) heterostructures and tuning their atomic and electronic structures is nowadays of particular interest due to the extraordinary properties and potential applications. Here, we demonstrate the temperature-induced phase-controlled growth of 1D Mo6Te6–2D MoTe2 heterostructures via molecular beam epitaxy. In situ scanning tunneling microscopy study shows 2D ultrathin films are synthesized at low temperature range, while 1D nanowires gradually arise and dominate as temperature increasing. X-ray photoelectron spectroscopy confirms the good stoichiometry and scanning tunneling spectroscopy reveals the semimetallic property of grown Mo6Te6 nanowires. Through in situ annealing, a phase transition from 2D MoTe2 to 1D Mo6Te6 is induced, thus forming a semimetal–semiconductor junction in atomic level. An upward band bending of 2H-MoTe2 is caused by lateral hole injection from Mo6Te6. The work suggests a new route to synthesize 1D semimetallic transit...

Journal ArticleDOI
TL;DR: In this article, a twisted trilayer graphene (TTG) with two different small twist angles between adjacent layers was systematically studied using scanning tunneling microscopy/spectroscopy (STM/STS).
Abstract: Twist, as a simple and unique degree of freedom, could lead to enormous novel quantum phenomena in bilayer graphene. A small rotation angle introduces low-energy van Hove singularities (VHSs) approaching the Fermi level, which result in unusual correlated states in the bilayer graphene. It is reasonable to expect that the twist could also affect the electronic properties of few-layer graphene dramatically. However, such an issue has remained experimentally elusive. Here, by using scanning tunneling microscopy/spectroscopy (STM/STS), we systematically studied a twisted trilayer graphene (TTG) with two different small twist angles between adjacent layers. Two sets of VHSs, originating from the two twist angles, were observed in the TTG, indicating that the TTG could be simply regarded as a combination of two different twisted bilayers of graphene. By using high-resolution STS, we observed a split of the VHSs and directly imaged the spatial symmetry breaking of electronic states around the VHSs. These results suggest that electron-electron interactions play an important role in affecting the electronic properties of graphene systems with low-energy VHSs.

Journal ArticleDOI
TL;DR: The introduction of Sn4+ in the (CH3NH3)3Sb2I9 structure has successfully lowered the pristine optical gap of the perovskite to a close-to optimum one and resulted in tuning of the type of electronic conductivity from p-type to n-type and more importantly led to a better band alignment with the selective contacts of p-i-n heterojunctions.
Abstract: The prevailing issue of wide optical gap in defect-ordered hybrid iodide perovskites has been addressed in this effort by heterovalent substitution at the metal site. With the introduction of Sn4+ in the (CH3NH3)3Sb2I9 structure, we have successfully lowered the pristine optical gap (2 eV) of the perovskite to a close-to optimum one (1.55 eV). Upon such heterovalent substitution, a gradual shift in the type of electronic conduction of the perovskites was observed. As evidenced from scanning tunneling spectroscopy and correspondingly density-of-state spectra, a significant shift of Fermi energy toward the conduction band edge occurred with an increase in the tin content in the host perovskite. This shift has resulted in tuning of the type of electronic conductivity from p-type to n-type and more importantly led to a better band alignment with the selective contacts of p–i–n heterojunctions. However, tin inclusion affected the surface roughness of the perovskite film in an adverse manner. Hence, the tin con...

Journal ArticleDOI
TL;DR: This work experimentally and theoretically study artificially enhanced spin-orbit coupling in graphene via random decoration with dilute Bi2Te3 nanoparticles to highlight a pathway to spintronics and quantum information applications in graphene-based quantum spin Hall platforms.
Abstract: Realization of the quantum-spin-Hall effect in graphene devices has remained an outstanding challenge dating back to the inception of the field of topological insulators. Graphene's exceptionally weak spin-orbit coupling -stemming from carbon's low mass- poses the primary obstacle. We experimentally and theoretically study artificially enhanced spin-orbit coupling in graphene via random decoration with dilute Bi2Te3 nanoparticles. Remarkably, multi-terminal resistance measurements suggest the presence of helical edge states characteristic of a quantum-spin-Hall phase; the magnetic-field and temperature dependence of the resistance peaks, X-ray photoelectron spectra, scanning tunneling spectroscopy, and first-principles calculations further support this scenario. These observations highlight a pathway to spintronics and quantum-information applications in graphene-based quantum-spin-Hall platforms.

Journal ArticleDOI
TL;DR: This work combines scanning tunneling spectroscopy with transport measurements to investigate the effect of nonmagnetic and magnetic substituents in SmB6, a predicted topological Kondo insulator and illustrates how magnetic impurities destroy the surface states from microscopic to macroscopic length scales.
Abstract: The impact of nonmagnetic and magnetic impurities on topological insulators is a central focus concerning their fundamental physics and possible spintronics and quantum computing applications. Combining scanning tunneling spectroscopy with transport measurements, we investigate, both locally and globally, the effect of nonmagnetic and magnetic substituents in SmB6, a predicted topological Kondo insulator. Around the so-introduced substitutents and in accord with theoretical predictions, the surface states are locally suppressed with different length scales depending on the substituent's magnetic properties. For sufficiently high substituent concentrations, these states are globally destroyed. Similarly, using a magnetic tip in tunneling spectroscopy also resulted in largely suppressed surface states. Hence, a destruction of the surface states is always observed close to atoms with substantial magnetic moment. This points to the topological nature of the surface states in SmB6 and illustrates how magnetic impurities destroy the surface states from microscopic to macroscopic length scales.

Journal ArticleDOI
30 Jul 2018-ACS Nano
TL;DR: It is shown that the energy gap between the first electronic tunneling resonances below and above the Fermi energy stabilizes to a finite value, determined by a first diradical electronic perturbative contribution to the polyacene electronic ground state.
Abstract: On-surface synthesis provides a powerful method for the generation of long acene molecules, making possible the detailed investigation of the electronic properties of single higher acenes on a surface. By means of scanning tunneling microscopy and spectroscopy combined with theoretical considerations, we discuss the polyradical character of the ground state of higher acenes as a function of the number of linearly fused benzene rings. We present energy and spatial mapping of the tunneling resonances of hexacene, heptacene, and decacene, and discuss the role of molecular orbitals in the observed tunneling conductance maps. We show that the energy gap between the first electronic tunneling resonances below and above the Fermi energy stabilizes to a finite value, determined by a first diradical electronic perturbative contribution to the polyacene electronic ground state. Up to decacene, the main contributor to the ground state of acenes remains the lowest-energy closed-shell electronic configuration.