On-Surface Synthesis of Nitrogen-Doped Kagome Graphene.

Nitrogen-doped Kagome graphene (N-KG) has been theoretically predicted as a candidate for the emergence of a topological band gap as well as unconventional superconductivity. However, its physical realization still remains very elusive. Here, we report on a substrate-assisted reaction on Ag(111) for the synthesis of two-dimensional graphene sheets possessing a long-range honeycomb Kagome lattice. Low-temperature scanning tunneling microscopy (STM) and atomic force microscopy (AFM) with a CO-terminated tip supported by density functional theory (DFT) are employed to scrutinize the structural and electronic properties of the N-KG down to the atomic scale. We demonstrate its semiconducting character due to the nitrogen doping as well as the emergence of Kagome flat bands near the Fermi level which would open new routes towards the design of graphene-based topological materials.

Proximity-Induced Superconductivity in Atomically Precise Nanographene on Ag/Nb(110).

Obtaining a robust superconducting state in atomically precise nanographene (NG) structures by proximity to a superconductor could foster the discovery of topological superconductivity in graphene. On-surface synthesis of such NGs has been achieved on noble metals and metal oxides; however, it is still absent on superconductors. Here, we present a synthetic method to induce superconductivity of polymeric chains and NGs adsorbed on the superconducting Nb(110) substrate covered by thin Ag films. Using atomic force microscopy at low temperature, we characterize the chemical structure of each subproduct formed on the superconducting Ag layer. Scanning tunneling spectroscopy further allows us to elucidate the electronic properties of these nanostructures, which consistently show a superconducting gap.

Strong signature of electron-vibration coupling in molecules on Ag(111) triggered by tip-gated discharging.

Electron-vibration coupling is of critical importance for the development of molecular electronics, spintronics, and quantum technologies, as it affects transport properties and spin dynamics. The control over charge-state transitions and subsequent molecular vibrations using scanning tunneling microscopy typically requires the use of a decoupling layer. Here we show the vibronic excitations of tetrabromotetraazapyrene (TBTAP) molecules directly adsorbed on Ag(111) into an orientational glassy phase. The electron-deficient TBTAP is singly-occupied by an electron donated from the substrate, resulting in a spin 1/2 state, which is confirmed by a Kondo resonance. The TBTAP•- discharge is controlled by tip-gating and leads to a series of peaks in scanning tunneling spectroscopy. These occurrences are explained by combining a double-barrier tunneling junction with a Franck-Condon model including molecular vibrational modes. This work demonstrates that suitable precursor design enables gate-dependent vibrational excitations of molecules on a metal, thereby providing a method to investigate electron-vibration coupling in molecular assemblies without a decoupling layer.

Topographic signatures and manipulations of Fe atoms, CO molecules and NaCl islands on superconducting Pb(111).

Topological superconductivity emerging in one- or two-dimensional hybrid materials is predicted as a key ingredient for quantum computing. However, not only the design of complex heterostructures is primordial for future applications but also the characterization of their electronic and structural properties at the atomic scale using the most advanced scanning probe microscopy techniques with functionalized tips. We report on the topographic signatures observed by scanning tunneling microscopy (STM) of carbon monoxide (CO) molecules, iron (Fe) atoms and sodium chloride (NaCl) islands deposited on superconducting Pb(111). For the CO adsorption a comparison with the Pb(110) substrate is demonstrated. We show a general propensity of these adsorbates to diffuse at low temperature under gentle scanning conditions. Our findings provide new insights into high-resolution probe microscopy imaging with terminated tips, decoupling atoms and molecules by NaCl islands or tip-induced lateral manipulation of iron atoms on top of the prototypical Pb(111) superconducting surface.

Atomically Precise Incorporation of BN-Doped Rubicene into Graphene Nanoribbons.

Substituting heteroatoms and non-benzenoid carbons into nanographene structure offers a unique opportunity for atomic engineering of electronic properties. Here we show the bottom-up synthesis of graphene nanoribbons (GNRs) with embedded fused BN-doped rubicene components on a Au(111) surface using on-surface chemistry. Structural and electronic properties of the BN-GNRs are characterized by scanning tunneling microscopy (STM) and atomic force microscopy (AFM) with CO-terminated tips supported by numerical calculations. The periodic incorporation of BN heteroatoms in the GNR leads to an increase of the electronic band gap as compared to its undoped counterpart. This opens avenues for the rational design of semiconducting GNRs with optoelectronic properties.