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We synthesize artificial graphene nanoribbons by positioning carbon monoxide molecules on a copper surface to confine its surface state electrons into artificial atoms positioned to emulate the low-energy electronic structure of graphene derivatives. We demonstrate that the dimensionality of artificial graphene can be reduced to one dimension with proper "edge" passivation, with the emergence of an effectively gapped one-dimensional nanoribbon structure. These one-dimensional structures show evidence of topological effects analogous to graphene nanoribbons. Guided by first-principles calculations, we spatially explore robust, zero-dimensional topological states by altering the topological invariants of quasi-one-dimensional artificial graphene nanostructures. The robustness and flexibility of our platform allow us to toggle the topological invariants between trivial and nontrivial on the same nanostructure. Ultimately, we spatially manipulate the states to understand fundamental coupling between adjacent topological states that are finely engineered and simulate complex Hamiltonians.

The ability to control nanoscale electronic properties by introducing macroscopic strain is of critical importance for the implementation of two-dimensional (2D) materials into flexible electronics...

Heterostructures of graphite/MoS2 display a wide range of lattice registry due to rotational alignment and/or lattice mismatch. Using high resolution scanning tunneling microscopy and spectroscopy (STM/STS) we investigated electronic properties of these heterostructures and observed changes in the bandgap as a function of the twist angle between the layers. Green's function based electronic structure calculations were carried out in order to shed light on the mechanism underlying the observed bandgap changes. Indirect coupling between the pz orbitals of the substrate Carbon atoms and the dz2 orbitals of the MoS2 layers (mediated by the pz orbitals of the bottom S layers) is found to be responsible for changes in the valence-band edge. Simple stacking of van der Waals materials with diverse properties have the potential to enable the fabrication of novel materials and device structures with tailored electronic properties. acceptedVersion

Using a q+ atomic force microscopy at low temperature, a sexiphenyl molecule is slid across an atomically flat Ag(111) surface along the direction parallel to its molecular axis and sideways to the axis. Despite identical contact area and underlying surface geometry, the lateral force required to move the molecule in the direction parallel to its molecular axis is found to be about half of that required to move it sideways. The origin of the lateral force anisotropy observed here is traced to the one-dimensional shape of the molecule, which is further confirmed by molecular dynamics simulations. We also demonstrate that scanning tunneling microscopy can be used to determine the comparative lateral force qualitatively. The observed one-dimensional lateral force anisotropy may have important implications in atomic scale frictional phenomena on materials surfaces.

Asymmetrical and dissymmetrical structures are widespread and play a critical role in nature and life systems. In the field of metallo-supramolecular assemblies, it is still in its infancy for constructing artificial architectures using dissymmetrical building blocks. Herein, we report the self-assembly of supramolecular systems based on two dissymmetrical double-layered ligands. With the aid of ultra-high-vacuum, low-temperature scanning tunneling microscopy (UHV-LT-STM), we were able to investigate four isomeric structures corresponding to four types of binding modes of ligand LA with two major conformations complexes A. The distribution of isomers measured by STM and total binding energy of each isomer obtained by density functional theory (DFT) calculations suggested that the most abundant isomer could be the most stable one with highest total binding energy. Finally, through shortening the linker between inner and outer layers and the length of arms, the arrangement of dissymmetrical ligand LB could be controlled within one binding mode corresponding to the single conformation for complexes B.

Topological phases of matter give rise to exotic physics that can be leveraged for next generation quantum computation1–3 and spintronic devices4,5. Thus, the search for topological phases and the quantum states that they exhibit have become the subject of a massive research effort in condensed matter physics. Topologically protected states have been produced in a variety of systems, including artificial lattices6–9, graphene nanoribbons (GNRs)10,11 and bismuth bilayers12,13. Despite these advances, the real-time manipulation of individual topological states and their relative coupling, a necessary feature for the realization of topological qubits, remains elusive. Guided by first-principles calculations, we spatially manipulate robust, zero-dimensional topological states by altering the topological invariants of quasi-one-dimensional artificial graphene nanostructures. This is achieved by positioning carbon monoxide molecules on a copper surface to confine its surface state electrons into artificial atoms positioned to emulate the low-energy electronic structure of graphene derivatives. Ultimately, we demonstrate control over the coupling between adjacent topological states that are finely engineered and simulate complex Hamiltonians. Our atomic synthesis gives access to an infinite range of nanoribbon geometries, including those beyond the current reach of synthetic chemistry, and thus provides an ideal platform for the design and study of novel topological and quantum states of matter.

We report on structural and electronic properties of defects in chemical vapor-deposited monolayer and few-layer MoS2 films. Scanning tunneling microscopy, Kelvin probe force microscopy, and transmission electron microscopy were used to obtain high resolution images and quantitative measurements of the local density of states, work function and nature of defects in MoS2 films. We track the evolution of defects that are formed under heating and electron beam irradiation. We observe formation of metastable domains with different work function values after annealing the material in ultra-high vacuum to moderate temperatures. We attribute these metastable values of the work function to evolution of crystal defects forming during the annealing. The experiments show that sulfur vacancies formed after exposure to elevated temperatures diffuse, coalesce, and migrate bringing the system from a metastable to equilibrium ground state. The process could be thermally or e-beam activated with estimated energy barrier for sulfur vacancy migration of 0.6 eV in single unit cell MoS2. Even at equilibrium conditions, the work function and local density of states values are strongly affected near grain boundaries and edges. The results provide initial estimates of the thermal budgets available for reliable fabrication of MoS2-based integrated electronics and indicate the importance of defect control and layer passivation.

Chemical vapor deposition has emerged as the most promising technique for the growth of graphene. However, most reports of this technique use either flammable or explosive gases, which bring safety concerns and extra costs to manage risk factors. In this article, we demonstrate that continuous monolayer graphene can be synthesized via chemical vapor deposition technique on Cu foils using industrially safe gas mixtures. Important factors, including the appropriate ratio of hydrogen flow and carbon precursor, pressure, and growth time are considered to obtain graphene films. Optical measurements and electrical transport measurements indicate graphene films are with comparable quality to other reports. Such continuous large area graphene can be synthesized under non-flammable and non-explosive conditions, which opens a safe and economical method for mass production of graphene. It is thereby beneficial for integration of graphene into semiconductor electronics.

Proximity effects in superconducting normal (SN) material heterostructures with metals and semiconductors have long been observed and theoretically described in terms of Cooper pair wave functions and Andreev reflections. Whereas the semiconducting

Low-temperature scanning tunneling microscopy and spectroscopy has been used to image the vortex core and the vortex lattice in FeSe single crystals. The local tunneling spectra acquired at the center of elliptical vortex cores display a strong particle-hole asymmetry with spatial oscillation, characteristic of the quantum-limit vortex core. Furthermore, a quasihexagonal vortex lattice at low magnetic field undergoes noticeable rhombic distortions above a certain field ∼1.5 T. This field H∗ also reveals itself as a kink in the magnetic field dependence of the specific heat. The observation of a nearly hexagonal vortex lattice at low field is very surprising for materials with an orthorhombic crystal structure and it is in apparent contradiction with the elliptical shape of the vortex cores. These observations can be directly connected to the multiband nature of superconductivity in this material, provided we attribute them to the suppression of superconducting order parameter in one of the energy bands. Above the field H∗ the superconducting coherence length for this band can well exceed the intervortex distance which strengthens the nonlocal effects. Therefore, in addition to multiple-band effects, other possible sources that can contribute to the observed evolution of the vortex-lattice structure include nonlocal effects which cause the field-dependent interplay between the symmetry of the crystal and vortex lattice or the magnetoelastic interactions due to the strain field generated by vortices. © 2019 American Physical Society. Citrus Research and Development Foundation, CRDF Government Council on Grants, Russian Federation Russian Science Foundation, RSF: 17-12-01383, 18-72-10027 Ministero dellâ Istruzione, dellâ Università e della Ricerca, MIUR Foundation for the Advancement of Theoretical Physics and Mathematics: 17-11-109 Ministero dellâ Istruzione, dellâ Università e della Ricerca, MIUR Kazan Federal University Office of Science, SC Division of Materials Sciences and Engineering, DMSE Russian Foundation for Basic Research, RFBR: 17-52-12044 Ministry of Education and Science of the Russian Federation, Minobrnauka Temple University, TU Argonne National Laboratory, ANL Nanjing University of Science and Technology, NUST: K2-2017-084 Drexel University The authors would like to acknowledge fruitful discussions with V. Kogan and T. Hanaguri. We also would like to acknowledge technical support during the early stage of these measurements from S. A. Moore. The work at Temple University, where low temperature scanning tunneling measurements were performed, was supported by US Department of Energy, Office of Science, Basic Energy Science, Materials Sciences and Engineering Division under Award No. DE-SC0004556. The work at Drexel University and at the M.V. Lomonosov Moscow State University was supported by the US Civilian Research and Development Foundation (CRDF Global). The work in Russia has been supported in part by the Ministry of Education and Science of the Russian Federation in the framework of the Increase Competitiveness Program of NUST MISiS Grant K2-2017-084, by Act 211 of the Government of Russian Federation, Contracts No. 02.A03.21.0004, No. 02.A03.21.0006, and No. 02.A03.21.0011 and by the Russian Government Program of Competitive Growth of Kazan Federal University. One of the authors (C.D.G.) would like to acknowledge partial support from MIUR (Ministry of Education, Universities and Research of the Italian Government). The work in IPM RAS (Nizhny Novgorod) was supported in part by the Russian Science Foundation (the calculation of the vortex-lattice characteristics Grant No. 18-72-10027; the calculation of the vortex-core deformation and the analysis of the experimental data Grant No. 17-12-01383), the Russian Foundation for Basic Research (Grant No. 17-52-12044), and Foundation for the Advancement of Theoretical Physics and Mathematics “BASIS” (Grant No. 17-11-109). The work at Argonne National Laboratory was supported by the US Department of Energy, Office of Science, Basic Energy Science, Materials Sciences and Engineering Division.

We report on structural and electronic properties of defects in chemical vapor-deposited monolayer and few-layer MoS2 films. We use scanning tunneling microscopy and Kelvin probe force microscopy in order to obtain measurements of the local density of states, work function and nature of defects in MoS2 films. We track the evolution of defects that are formed under annealing in ultra-high vacuum conditions. We observe formation of metastable domains with different work function values after annealing the material in ultra-high vacuum to moderate temperatures. We attribute these metastable values of the work function to evolution of crystal defects forming during the annealing. The experiments show that sulfur vacancies formed after exposure to elevated temperatures diffuse, coalesce, and migrate bringing the system from a metastable to equilibrium ground state. The process could be thermally activated with estimated energy barrier for sulfur vacancy migration of 0.6 eV in single unit cell MoS2. The results provide estimates of the thermal budgets available for reliable fabrication of MoS2-based integrated circuit electronics and indicate the importance of defect control and layer passivation.We report on structural and electronic properties of defects in chemical vapor-deposited monolayer and few-layer MoS2 films. We use scanning tunneling microscopy and Kelvin probe force microscopy in order to obtain measurements of the local density of states, work function and nature of defects in MoS2 films. We track the evolution of defects that are formed under annealing in ultra-high vacuum conditions. We observe formation of metastable domains with different work function values after annealing the material in ultra-high vacuum to moderate temperatures. We attribute these metastable values of the work function to evolution of crystal defects forming during the annealing. The experiments show that sulfur vacancies formed after exposure to elevated temperatures diffuse, coalesce, and migrate bringing the system from a metastable to equilibrium ground state. The process could be thermally activated with estimated energy barrier for sulfur vacancy migration of 0.6 eV in single unit cell MoS2. The results...

Single crystals of sulfur-substituted iron selenide, FeSe1-xSx, were grown within eutectics of molten halides, AlCl3/KCl, AlCl3/KCl/NaCl or AlCl3/KBr, under permanent temperature gradient. The innovative "ampoule in ampoule" design of a crystallization vessel allows obtaining mm-sized plate-like single crystals with a sulfur content up to x ∼ 0.19. The sharp anomalies in the physical properties indicate the superconducting and nematic phase transitions in FeSe0.96 at TC = 8.4 K and TN = 90 K, respectively. Scanning tunneling microscopy reveals the presence of dumbbell defects associated with Fe vacancies and dark defects at the chalcogen site associated with S within the FeSe1-xSx series of compounds. Scanning tunneling spectroscopy shows the presence of two different superconducting gaps at both hole and electron pockets of the Fermi surface for low S content levels. As a function of sulfur content, TC follows the conventional dome-shaped curve while TN decreases with x. The overall appearance of the T-x phase diagram of FeSe1-xSx suggests the importance of nematic fluctuations for the formation of the superconducting state in these compounds. © 2018 The Royal Society of Chemistry.

Recent progress in the synthesis of monolayer MoS2, a two-dimensional direct band-gap semiconductor, is paving new pathways toward atomically thin electronics. Despite the large amount of literature, fundamental gaps remain in understanding electronic properties at the nanoscale. Here, we report a study of highly crystalline islands of MoS2 grown via a refined chemical vapor deposition synthesis technique. Using high resolution scanning tunneling microscopy and spectroscopy (STM/STS), photoemission electron microscopy/spectroscopy (PEEM) and μ-ARPES we investigate the electronic properties of MoS2 as a function of the number of layers at the nanoscale and show in-depth how the band gap is affected by a shift of the valence band edge as a function of the layer number. Green’s function based electronic structure calculations were carried out in order to shed light on the mechanism underlying the observed bandgap reduction with increasing thickness, and the role of the interfacial Sulphur atoms is clarified. Our study, which gives new insight into the variation of electronic properties of MoS2 films with thickness bears directly on junction properties of MoS2, and thus impacts electronics application of MoS2.

Recent progress in the synthesis of monolayer MoS2, a two-dimensional direct band-gap semiconductor, is paving new pathways toward atomically thin electronics. Despite the large amount of literature, fundamental gaps remain in understanding electronic properties at the nanoscale. Here, we report a study of highly crystalline islands of MoS2 grown via a refined chemical vapor deposition synthesis technique. Using high resolution scanning tunneling microscopy and spectroscopy (STM/STS), photoemission electron microscopy/spectroscopy (PEEM) and μ-ARPES we investigate the electronic properties of MoS2 as a function of the number of layers at the nanoscale and show in-depth how the band gap is affected by a shift of the valence band edge as a function of the layer number. Green’s function based electronic structure calculations were carried out in order to shed light on the mechanism underlying the observed bandgap reduction with increasing thickness, and the role of the interfacial Sulphur atoms is clarified. Our study, which gives new insight into the variation of electronic properties of MoS2 films with thickness bears directly on junction properties of MoS2, and thus impacts electronics application of MoS2.

Scanning tunneling spectroscopy has been used to investigate the superconducting gaps of FeSe 1−x S x single crystals and to reveal signatures of a bosonic mode in the quasiparticle density of states. We find that both superconducting gaps residing on different pockets of the Fermi surface are anisotropic. Moreover, the bosonic mode appears in the quasiparticle density of states as a redistribution of states at energy Ω/e, measured with respect to the superconducting gap. The energy of the boson mode Ω is found to scale with the superconducting gap, and it can be estimated to be in the range 2.6 ÷ 3.8 meV in agreement with a recent observation of a resonance spin excitation in neutron scattering. This suggests that quasiparticle interactions with this mode are important for superconductivity.

An insulating barrier is one of the key components in electronic devices that makes use of quantum tunneling principles. Many metal-oxides have been used as a good barrier material in a tunnel junction for their large band gap, stable chemical properties and superb properties for forming a thin and pin-hole-free insulating layer. The reduced dimensions of transistors have led to the need for alternative, high dielectric constant (high-κ) oxides to replace conventional silicon-based dielectrics to reduce the leaking current induced by electron tunneling. On the other hand, a tunnel junction with one or both electrodes made of graphene may lead to novel applications due to the massless Dirac fermions from the graphene. Here we have fabricated sandwich-type graphene tunnel junctions with high-κ metal-oxides as barriers, including Al2O3, HfO2, ZrO2, and TiO2. Tunneling properties are investigated by observing the temperature and time dependences of the tunneling spectra. Our results show the potential for applications of high-κ oxides in graphene tunnel junctions and bringing new opportunities for memory and logic electronic devices.

We report a development of graphene tunnel junctions made by chemical vapor deposition grown graphene and sputtered aluminum insulating by an in-situ grown aluminum oxide. The thin oxide layer formed in between the metal layer and the two-dimensional material is a crucial part of a tunnel junction. We characterized surface morphology of oxide layers and studied tunneling spectra of lead and silver tunnel junctions to estimate the quality of the aluminum oxide. The Brinkman-Rowell-Dynes model was applied to fit the conductance-voltage plots to calculate the thickness of oxide layers. Junctions with graphene both on bottom and on top were fabricated and their tunneling properties were characterized after exposure to air for weeks to test time stability. Furthermore, the resistances of graphene tunnel junctions with aluminum oxide formed naturally and in an oxygen atmosphere were studied. Our results demonstrate that in-situ aluminum oxide is an effective barrier for graphene tunnel junctions. The methods of...