Quasi-Periodic Growth of One-Dimensional Copper Boride on Cu(110).

An unexplored material of copper boride has been realized recently in two-dimensional form at a (111) surface of the fcc copper crystal. Here, one-dimensional (1-D) boron growth was observed on the Cu(110) surface, as probed by atomically resolved scanning probe microscopy. The 1-D copper boride was composed of quasi-periodic atomic chains periodically aligned parallel to each other, as confirmed by Fourier transform analysis. The 1-D growth unexpectedly proceeded across surface steps in a self-assembled manner and extended over several 100 nm. The long-range formation of a 1-D quasi-periodic structure on a surface has been theoretically modeled as a 1-D quasi-crystal and the predicted conditions matched the structural parameters obtained by the experimental work here. The quasi-periodic 1-D copper boride system enabled a way to examine 1-D quasi-crystallinity on an actual material.

Revealing the Hidden Spin-Polarized Bands in a Superconducting Tl Bilayer Crystal.

The interplay of spin-orbit coupling and crystal symmetry can generate spin-polarized bands in materials only a few atomic layers thick, potentially leading to unprecedented physical properties. In the case of bilayer materials with global inversion symmetry, locally broken inversion symmetry can generate degenerate spin-polarized bands, in which the spins in each layer are oppositely polarized. Here, we demonstrate that the hidden spins in a Tl bilayer crystal are revealed by growing it on Ag(111) of sizable lattice mismatch, together with the appearance of a remarkable phenomenon unique to centrosymmetric hidden-spin bilayer crystals: a novel band splitting in both spin and space. The key to success in observing this novel splitting is that the interaction at the interface has just the right strength: it does not destroy the original wave functions of the Tl bilayer but is strong enough to induce an energy separation.

Squeezed Abrikosov-Josephson Vortex in Atomic-Layer Pb Superconductors Formed on Vicinal Si(111) Substrates.

Unlike bulk counterparts, two-dimensional (2D) superconductors are sensitive to disorder. Here, we investigated superconductivity of Pb atomic layers formed on vicinal substrates to reveal how surface steps with an interval shorter than the coherence length ξ affect it. Electrical transport showed reduced critical temperature and enhanced critical magnetic field. Scanning tunneling microscopy exhibited vortices elongated along the steps, that is, Abrikosov-Josephson vortices squeezed normal to the steps due to the reduced ξ. These results demonstrate that steps work as disorder and vicinal substrates provide a unique platform to manipulate the degree of disorder on 2D superconductors.

Dirac Fermions in Borophene.

Honeycomb structures of group IV elements can host massless Dirac fermions with nontrivial Berry phases. Their potential for electronic applications has attracted great interest and spurred a broad search for new Dirac materials especially in monolayer structures. We present a detailed investigation of the ß_{12} sheet, which is a borophene structure that can form spontaneously on a Ag(111) surface. Our tight-binding analysis revealed that the lattice of the ß_{12} sheet could be decomposed into two triangular sublattices in a way similar to that for a honeycomb lattice, thereby hosting Dirac cones. Furthermore, each Dirac cone could be split by introducing periodic perturbations representing overlayer-substrate interactions. These unusual electronic structures were confirmed by angle-resolved photoemission spectroscopy and validated by first-principles calculations. Our results suggest monolayer boron as a new platform for realizing novel high-speed low-dissipation devices.

Electrical Conductivity through a Single Atomic Step Measured with the Proximity-Induced Superconducting Pair Correlation.

Local disordered nanostructures in an atomically thick metallic layer on a semiconducting substrate play significant and decisive roles in transport properties of two-dimensional (2D) conductive systems. We measured the electrical conductivity through a step of monoatomic height in a truly microscopic manner by using as a signal the superconducting pair correlation induced by the proximity effect. The transport property across a step of a one-monolayer Pb surface metallic phase, formed on a Si(111) substrate, was evaluated by inducing the pair correlation around the local defect and measuring its response, i.e., the reduced density of states at the Fermi energy using scanning tunneling microscopy. We found that the step resistance has a significant contribution to the total resistance on a nominally flat surface. Our study also revealed that steps in the 2D metallic layer terminate the propagation of the pair correlation. Superconductivity is enhanced between the first surface step and the superconductor-normal-metal interface by reflectionless tunneling when the step is located within a coherence length.

Site-Dependent Evolution of Electrical Conductance from Tunneling to Atomic Point Contact.

Using scanning tunneling microscopy (STM), we investigated the evolution of electrical conductance between a Pb tip and Pb(111) surface from tunneling to atomic point contact at a site that was defined with atomic precision. We found that the conductance evolution depended on the contact site, for instance, on-top, bridge, or hollow (hcp and fcc) sites in the Pb lattice. In the transition from tunneling to contact regimes, the conductance measured at the on-top site was enhanced. In the point contact regime, the hollow sites had conductances larger than those of the other sites, and between the hollow sites, the hcp site had a conductance larger than that of the fcc site. We also observed the enhancement and reversal of the apparent height in atomically resolved high-current STM images, consistent with the results of the conductance traces. Our results indicate the importance of atomic configuration in the conductance of atomic junctions and suggest that attractive chemical interactions have a significant role in electron transport between contacting atoms.

Imaging Josephson vortices on the surface superconductor Si(111)-(√7×√3)-In using a scanning tunneling microscope.

We have studied the superconducting Si(111)-(√7×√3)-In surface using a ³He-based low-temperature scanning tunneling microscope. Zero-bias conductance images taken over a large surface area reveal that vortices are trapped at atomic steps after magnetic fields are applied. The crossover behavior from Pearl to Josephson vortices is clearly identified from their elongated shapes along the steps and significant recovery of superconductivity within the cores. Our numerical calculations combined with experiments clarify that these characteristic features are determined by the relative strength of the interterrace Josephson coupling at the atomic step.

Scanning tunneling microscopy/spectroscopy of picene thin films formed on Ag(111).

Using ultrahigh-vacuum low-temperature scanning tunneling microscopy and spectroscopy combined with first principles density functional theory calculations, we have investigated structural and electronic properties of pristine and potassium (K)-deposited picene thin films formed in situ on a Ag(111) substrate. At low coverages, the molecules are uniformly distributed with the long axis aligned along the [112̄] direction of the substrate. At higher coverages, ordered structures composed of monolayer molecules are observed, one of which is a monolayer with tilted and flat-lying molecules resembling a (11̄0) plane of the bulk crystalline picene. Between the molecules and the substrate, the van der Waals interaction is dominant with negligible hybridization between their electronic states; a conclusion that contrasts with the chemisorption exhibited by pentacene molecules on the same substrate. We also observed a monolayer picene thin film in which all molecules were standing to form an intermolecular π stacking. Two-dimensional delocalized electronic states are found on the K-deposited π stacking structure.

Metallic transport in a monatomic layer of in on a silicon surface.

We have succeeded in detecting metallic transport in a monatomic layer of In on an Si(111) surface, Si(111)-sqrt[7]×sqrt[3]-In surface reconstruction, using the micro-four-point probe method. The In layer exhibited conductivity higher than the minimum metallic conductivity (the Ioffe-Regel criterion) and kept the metallic temperature dependence of resistivity down to 10 K. This is the first example of a monatomic layer, with the exception of graphene, showing metallic transport without carrier localization at cryogenic temperatures. By introducing defects on this surface, a metal-insulator transition occurred due to Anderson localization, showing hopping conduction.

Reduction in magnetic coercivity of Co nanomagnets by Fe alloying.

We measured the magnetic hysteresis and coercivity of individual Co and Co0.8Fe0.2 bilayer nano-sized island structures formed on Cu (111) substrate using spin-polarized scanning tunneling microscopy. From the hysteresis taken on various sizes of islands, we found that the alloyed islands are ferromagnetic with out-of-plane magnetic anisotropy, same as the pure islands. Coercivity of the alloy islands, which is dependent on their size, was significantly reduced to ≈40% of that of the pure islands. Based on the Stoner-Wohlfarth model, we evaluated the amount of magnetic anisotropic energy and anisotropy constant for both pure and alloy islands. Since tunneling spectra taken on the alloy islands show upward shifts of the valence electronic states as compared to the pure ones, fewer electrons populated in the valence band of the alloy islands are presumably responsible for the reduction in the magnetic anisotropic energy.

Tip-induced excitation of a single vortex in nano-size superconductors using scanning tunneling microscopy.

A single vortex is excited into nano-size Pb superconducting island structures by a local current injection from a probe tip of a scanning tunneling microscope. For the excitation, a sufficient amount and duration of the pulsed current are required. Injecting the current at peripheral sites is more effective than the center for the vortex excitation. Time-dependent Ginzburg-Landau calculations suggest that a current-induced normal-state area, which can be nucleated by the tunneling current exceeding the critical current and expanded by the Joule heating, reduces the required magnetic field for the vortex penetration and excites a vortex into the islands.

Scanning tunneling microscopy on cleaved Mn3Sn(0001) surface.

We have studied in-situ cleaved (0001) surfaces of the magnetic Weyl semimetal Mn3Sn by low-temperature scanning tunneling microscopy and spectroscopy (STM/S). It was found that freshly cleaved Mn3Sn surfaces are covered with unknown clusters, and the application of voltage pulses in the tunneling condition was needed to achieve atomically flat surfaces. STM topographs taken on the flat terrace show a bulk-terminated 1 × 1 honeycomb lattice with the Sn site brightest. First-principles calculations reveal that the brightest contrast at the Sn site originates from the surrounding surface Mn d orbitals. Tunneling spectroscopy performed on the as-cleaved and voltage-pulsed surfaces show a prominent semimetal valley near the Fermi energy.

Bulk ferromagnetic tips for spin-polarized scanning tunneling microscopy.

We characterized the performance of electrochemically etched bulk Fe and Ni tips as a probe of spin-polarized scanning tunneling microscopy (SP-STM). Through the observation of the striped contrast on the conical spin-spiral structure formed in Mn double layers on a W(110) substrate, the capability of both the tips to detect the magnetic signal was clarified. We also confirmed that the magnetized direction of the Fe and Ni tips can be flipped between the two out-of-plane directions by external magnetic fields. Our results demonstrate that the ex-situ prepared tips are reliable in SP-STM for the samples that are not susceptible to a stray magnetic field.

Atomically resolved imaging by low-temperature frequency-modulation atomic force microscopy using a quartz length-extension resonator.

Low-temperature ultrahigh vacuum frequency-modulation atomic force microscopy (AFM) was performed using a 1 MHz length-extension type of quartz resonator as a force sensor. Taking advantage of the high stiffness of the resonator, the AFM was operated with an oscillation amplitude smaller than 100 pm, which is favorable for high spatial resolution, without snapping an AFM tip onto a sample surface. Atomically resolved imaging of the adatom structure on the Si(111)-(7x7) surface was successfully obtained.

Experimental verification of the rotational type of chiral spin spiral structures by spin-polarized scanning tunneling microscopy.

We report on experimental verification of the rotational type of chiral spin spirals in Mn thin films on a W(110) substrate using spin-polarized scanning tunneling microscopy (SP-STM) with a double-axis superconducting vector magnet. From SP-STM images using Fe-coated W tips magnetized to the out-of-plane and [001] directions, we found that both Mn mono- and double-layers exhibit cycloidal rotation whose spins rotate in the planes normal to the propagating directions. Our results agree with the theoretical prediction based on the symmetry of the system, supporting that the magnetic structures are driven by the interfacial Dzyaloshinskii-Moriya interaction.

Atomic-scale visualization of surface-assisted orbital order.

Orbital-related physics attracts growing interest in condensed matter research, but direct real-space access of the orbital degree of freedom is challenging. We report a first, real-space, imaging of a surface-assisted orbital ordered structure on a cobalt-terminated surface of the well-studied heavy fermion compound CeCoIn5. Within small tip-sample distances, the cobalt atoms on a cleaved (001) surface take on dumbbell shapes alternatingly aligned in the [100] and [010] directions in scanning tunneling microscopy topographies. First-principles calculations reveal that this structure is a consequence of the staggered d xz -d yz orbital order triggered by enhanced on-site Coulomb interaction at the surface. This so far overlooked surface-assisted orbital ordering may prevail in transition metal oxides, heavy fermion superconductors, and other materials.

Guided Molecular Assembly on a Locally Reactive 2D Material.

Atomically precise engineering of the position of molecular adsorbates on surfaces of 2D materials is key to their development in applications ranging from catalysis to single-molecule spintronics. Here, stable room-temperature templating of individual molecules with localized electronic states on the surface of a locally reactive 2D material, silicene grown on ZrB2 , is demonstrated. Using a combination of scanning tunneling microscopy and density functional theory, it is shown that the binding of iron phthalocyanine (FePc) molecules is mediated via the strong chemisorption of the central Fe atom to the sp3 -like dangling bond of Si atoms in the linear silicene domain boundaries. Since the planar Pc ligand couples to the Fe atom mostly through the in-plane d orbitals, localized electronic states resembling those of the free molecule can be resolved. Furthermore, rotation of the molecule is restrained because of charge rearrangement induced by the bonding. These results highlight how nanoscale changes can induce reactivity in 2D materials, which can provide unique surface interactions for enabling novel forms of guided molecular assembly.

Nanoscale chemical imaging by scanning tunneling microscopy assisted by synchrotron radiation.

Nanoscale chemical imaging using scanning tunneling microscopy is demonstrated with a core-level excitation of the probed element by a synchrotron radiation light. Pronounced element-specific contrasts were observed in the spatial resolution of approximately 10 nm on checkerboard-patterned Ni and Fe samples in differential photoinduced current images taken with the scanning tunneling microscopy tip under the synchrotron radiation irradiation whose photon energies are above and below the Ni (Fe) L absorption edge. The local detection of the photoinduced secondary electrons through the surface barrier lowered by the proximate tip and/or via the tunneling process probably plays an important role in achieving the high-spatial resolution.

Superconducting Pb island nanostructures studied by scanning tunneling microscopy and spectroscopy.

Superconductivity of nanosized Pb-island structures whose radius is 0.8 to 2.5 times their coherence length was studied under magnetic fields using low-temperature scanning tunneling microscopy and spectroscopy. Spatial profiles of superconductivity were obtained by conductance measurements at zero-bias voltage. Critical magnetic fields for vortex penetration and expulsion and for superconductivity breaking were measured for each island. The critical fields depending on the lateral size of the islands and existence of the minimum lateral size for vortex formation were observed.

Adsorption, manipulation and self-assembling of TBrPP-Co molecules on a Ag/Si(111) surface by scanning tunnelling microscopy.

Individual adsorption and two-dimensional assembling of 5,10,15,20-tetrakis-(4-bromophenyl)-porphyrin-Co (TBrPP-Co) molecules on a Si(111)-[Formula: see text] Ag reconstructed surface have been studied using low-temperature scanning tunnelling microscopy (STM). All the isolated molecules are observed in a planar shape with slight distortion. The isolated molecules can be controllably rotated with an STM tip to the orientation along the trigonal lattice ([Formula: see text] direction) of the substrate. With an increased coverage (0.07 ML) and appropriate annealing, the molecules assemble to form three types of ordered phase. The long-range ordered structures, however, disappear at higher coverage (0.75 ML).