Locally varying formation of nanoclusters across a low-intensity ultra-short laser spot.

Ultra-short laser illumination is an intriguing tool for engineering material by light. It is usually employed at or above the ablation threshold. Practical applications profit from tailoring surface properties, for instance, by structural changes to the surface layer of an irradiated target. A target-orientated restructuring of surfaces on the nanoscale is much less explored. In particular, an intrinsic intensity variation across a laser spot has not yet been considered or employed. We image the unexpected nanoscale clusters formed on the Cu(111) surface upon illumination of a Cu sample far below its ablation threshold by femtosecond laser light, employing a specifically-developed multi-scale approach. We unravel that these clusters vary significantly in size and shape across the micrometer-scale 400 nm 50 fs laser spot (repetition rate: 250 kHz). There are three qualitatively different regions separated by sharp changes. The observations highlight the importance of local fluence for specific types of nanoclusters. Ultra-short laser illumination represents a non-trivial interplay between photo-thermal and electron-induced mechanisms, transport of heat and electrons, and material properties, which we discuss for identifying the underlying principles. Our study demonstrates that a multitude of as yet unconsidered processes are involved in the tailoring of nanoscale materials by ultra-short laser light.

Moiré Superlattice-Induced Superconductivity in One-Unit-Cell FeTe.

In this work, we demonstrate that the nonsuperconducting single-layer FeTe can become superconducting when its structure is properly tuned by epitaxially growing it on Bi2Te3 thin films. The properties of the single-layer FeTe deviate strongly from its bulk counterpart, as evidenced by the emergence of a large superconductivity gap (3.3 meV) and an apparent 8 × 2 superlattice (SL). Our first-principles calculations indicate that the 8 × 2 SL and the emergence of the novel superconducting phase are essentially the result of the structural change in FeTe due to the presence of the underlying Bi2Te3 layer. The structural change in FeTe likely suppresses the antiferromagnetic order in the FeTe and leads to superconductivity. Our work clearly demonstrates that moiré pattern engineering in a heterostructure is a reachable dimension for investigating novel materials and material properties.

Superconductivity in Single-Quintuple-Layer Bi2Te3 Grown on Epitaxial FeTe.

How an interfacial superconductivity emerges during the nucleation and epitaxy is of great importance not only for unveiling the physical insights but also for finding a feasible way to tune the superconductivity via interfacial engineering. In this work, we report the nanoscale creation of a robust and relatively homogeneous interfacial superconductivity (TC ≈ 13 K) on the epitaxial FeTe surface, by van der Waals epitaxy of single-quintuple-layer topological insulator Bi2Te3. Our study suggests that the superconductivity in the Bi2Te3/FeTe heterostructure is generated at the interface and that the superconductivity at the interface does not enhance or weaken with the increase of the Bi2Te3 thickness beyond 1 quintuple layer (QL). The observation of the topological surface states crossing Fermi energy in the Bi2Te3/FeTe heterostructure with the average Bi2Te3 thickness of about 20 QL provides further evidence that this heterostructure may potentially host Majorana zero modes.

Non-local atomic manipulation on semiconductor surfaces in the STM: the case of chlorobenzene on Si(111)-7×7.

Control over individual atoms with the scanning tunnelling microscope (STM) holds the tantalising prospect of atomic-scale construction, but is limited by its "one atom at a time" serial nature. "Remote control" through non-local STM manipulation-as we have demonstrated in the case of chlorobenzene on Si(111)-7×7-offers a new avenue for future "bottom-up" nanofabrication, since hundreds of chemical reactions may be carried out in parallel. Thus a good understanding of the non-local manipulation process, as provided by recent experiments, is important. Comparison of scanning tunnelling spectroscopy (STS) measurements of the bare Si(111)-7×7 surface and chemisorbed chlorobenzene molecules with the voltage dependence of the non-local STM-induced desorption of chlorobenzene proves particularly instructive. For example, the chlorobenzene LUMO appears at +0.9 V with respect to the Fermi level, whereas non-local manipulation thresholds are found at +2.1 V and +2.7 V. This difference supports a picture in which the voltage thresholds for non-local electron-induced desorption depend principally on the energies of the electronic states of the surface. Furthermore, the demonstration that the non-local process is largely insensitive to surface steps up to five layers in height suggests that either the electron transport in this process is subsurface in character or surface charge transport is responsible but is in some way unaffected by the steps.

Quantum chemical cluster models for chemi- and physisorption of chlorobenzene on Si(111)-7×7.

Motivated by recent atomic manipulation experiments, we report quantum chemical calculations for chemi- and physisorption minima of chlorobenzene on the Si(111)-7×7 surface. A density functional theory cluster approach is applied, using the B3LYP hybrid functional alongside Grimme's empirical dispersion corrections (D3). We were able to identify chemisorption sites of binding energies of 1.6 eV and physisorption energies of 0.6 eV, both in encouraging agreement with the trend of experimental data. The cluster approach opens up the possibility of a first-principles based dynamical description of STM manipulation experiments on this system, the interpretation of which involves both the chemi- and physisorbed states. However, we found that special care has to be taken regarding the choice of clusters, basis sets, and the evaluation of the dispersion corrections.