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

Observation of robust superlubricity of MoS₂ on Au(111) in ultrahigh vacuum

The structural and superlubric properties of single layer MoS2 on Au(1 1 1) forming moiré superlattice structures have been investigated by means of ultrahigh vacuum atomic force microscope with bimodal and contact modes. We synthesize epitaxial monolayer MoS2 flakes on the Au(1 1 1) surface in ultrahigh vacuum. Using friction force microscopy, atomic friction measurements indicate a superlubric regime between the tip apex and the moiré corrugated MoS2 surface in which the friction force remains at an ultralow value and is independent from normal load. Superlubricity conditions are observed for different loads and velocities which indicates the absence of out-of-plane deformations. We find that the MoS2 layer including the moiré superlattice modulation originating from the natural misfit between MoS2 and the Au(1 1 1) substrate is relatively rigid. We also demonstrate a low friction coefficient of the MoS2 surface crossing a single Au(1 1 1) step. Our results open up a new avenue for minimizing friction in nanoscale electronic devices and other dry rigid contacts used in aerospace lubrication

Polygonal tessellations as predictive models of molecular monolayers

Molecular self-assembly plays a very important role in various aspects of technology as well as in biological systems. Governed by the covalent, hydrogen or van der Waals interactions - self-assembly of alike molecules results in a large variety of complex patterns even in two dimensions (2D). Prediction of pattern formation for 2D molecular networks is extremely important, though very challenging, and so far, relied on computationally involved approaches such as density functional theory, classical molecular dynamics, Monte Carlo, or machine learning. Such methods, however, do not guarantee that all possible patterns will be considered and often rely on intuition. Here we introduce a much simpler, though rigorous, hierarchical geometric model founded on the mean-field theory of 2D polygonal tessellations to predict extended network patterns based on molecular-level information. Based on graph theory, this approach yields pattern classification and pattern prediction within well-defined ranges. When applied to existing experimental data, our model provides an entirely new view of self-assembled molecular patterns, leading to interesting predictions on admissible patterns and potential additional phases. While developed for hydrogen-bonded systems, an extension to covalently bonded graphene-derived materials or 3D structures such as fullerenes is possible, significantly opening the range of potential future applications

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

Abstract 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

Flexible superlubricity unveiled in sidewinding motion of individual polymeric chains

A combination of low temperature atomic force microcopy and molecular dynamic simulations is used to demonstrate that soft designer molecules realize a sidewinding motion when dragged over a gold surface. Exploiting their longitudinal flexibility, pyrenylene chains are indeed able to lower diffusion energy barriers via on-surface directional locking and molecular strain. The resulting ultralow friction reaches values on the order of tens of pN reported so far only for rigid chains sliding on an incommensurate surface. Therefore, we demonstrate how molecular flexibility can be harnessed to realize complex nanomotion while retaining a superlubric character. This is in contrast with the paradigm guiding the design of most superlubric nanocontacts (mismatched rigid contacting surfaces

Gate-tunable topological superconductivity in a supramolecular electron spin lattice

Topological superconductivity emerges in chains or arrays of magnetic atoms coupled to a superconductor. However, the external controllability of such systems with gate voltages is detrimental for their future implementation in a topological quantum computer. Here we showcase the supramolecular assembly of radical molecules on Pb(111), whose discharge is controlled by the tip of a scanning tunneling microscope. Charged molecules carry a spin-1/2 state, as confirmed by observing Yu-Shiba-Rusinov in-gap states by tunneling spectroscopy at millikelvin temperature. Low energy modes are localized at island boundaries with a long decay towards the interior, whose spectral signature is consistent with Majorana zero modes protected by mirror symmetry. Our results open up a vast playground for the synthesis of gate-tunable organic topological superconductors

Design and Characterization of an Electrically Powered Single Molecule on Gold

The surface diffusion of individual molecules is of paramount importance in self-assembly processes and catalytic processes. However, the fundamental understanding of molecule diffusion peculiarities considering conformations and adsorption sites remain poorly known at the atomic scale. Here, we probe the 4′-(4-tolyl)-2,2′:6′,2″-terpyridine adsorbed on the Au(111) herringbone structure combining scanning tunneling microscopy and atomic force microscopy. Molecules are controllably translated by electrons excitations over the reconstruction, except at elbows acting as pinning centers. Experimental data supported by theoretical calculations show the formation of coordination bonds between the molecule and Au atoms of the surface. Using force spectroscopy, we quantify local variation of the surface potential and the lateral force required to move the molecule. We found an elevation of the diffusion barrier at elbows of the reconstruction of ∼100 meV compared to the rest of the surface

Auto-assemblage et polymérisation 2D de molécules organiques en surface

This work deals with the investigation under ultra high vacuum of organic monolayers either resulting from the self-assembly or from the polymerization of individual molecular building blocks (hexahydroxy triphenylene-HHTP and diboronic acid-BDBA) at the surface of a metal and an insulator. By means of scanning tunneling microscopy (STM), we have shown that HHTP molecules condense on Ag(111) into distinct supramolecular phases depending on the substrate temperature. A robust network can be obtained by partial dehydrogenation of the peripheral alcohol groups of HHTP, hence yielding H-bonds between the newly formed quinone groups and the alcohol groups remaining intact. STM studies of BDBA on Ag(111) revealed an organic network resulted from the creation of covalent bonds between BDBA molecules, by a two-dimensional polymerization confined on surface. On the same surface, another kind of surface covalent organic framework (SCOF) was also evidenced by copolymerization between HHTP and BDBA molecules. The SCOF's exhibits a well-extended bidimensional character with an exceptional thermal stability. Finally, the study by non-contact atomic force microscopy (nc-AFM) of BDBA on KCl(001) has shown a bi-dimensional and well-extended phase stabilized by intermolecular H-bonds. The latter example evidences the in uence of the chemical nature of the substrate to initiate the 2D-polymerization process on surface. Our results suggest that the use of chemical reactions at surfaces opens up a new approach for the development of robust and original molecular architectures.Ce travail présente la formation et la caractérisation sous ultravide de monocouches moléculaires issu de l'auto-assemblage et de la polymérisation de molécules organiques (hexahydroxy triphenyléne-HHTP et acide diborique benzoique-BDBA) sur des surfaces monocristallines métalliques et isolantes. L'adsorption de molécules HHTP sur Ag(111) donne lieu à plusieurs réseaux moléculaires dépendants de la température. Cette étude, menée par microscopie à effet tunnel (STM), montre qu'un réseau robuste est obtenu suite à la déshydrogénation, activée thermiquement, des groupes alcool périphériques. Cela induit la formation de liaisons hydrogène entre les fonctions alcools et cétones ainsi obtenues. L'étude STM de molécules de BDBA vapo-déposées sur Ag(111) a démontrée la formation d'architectures bidimensionnelles étendues, liées de manière covalente, suite à la polymérisation des précurseurs en surface. Un résultat similaire a pu être obtenu par la copolymérisation des molécules de BDBA et d'HHTP. Ces polymères nanoporeux s'étendent en monocouche et présentent une stabilité en température exceptionnelle. Enfin, l'étude de BDBA sur le substrat isolant de KCl, menée par microscopie à force atomique en mode non contact (nc-AFM), montre un auto-assemblage étendu par des liaisons hydrogène, et met en évidence le rôle décisif de la nature chimique du substrat sur la faisabilité de la polymérisation de ces molécules en surface. L'approche développée dans ce travail, mettant en jeu des réactions chimiques en surface, constitue une voie nouvelle pour la conception de nano-architectures moléculaires originales et robustes sur surfaces

Atomically Precise Incorporation of BN-Doped Rubicene into Graphene Nanoribbons

<p>Raw file of publication entitled "Atomically Precise Incorporation of BN-Doped Rubicene into Graphene Nanoribbons"</p><p>https://doi.org/10.1021/acs.jpcc.2c05866</p&gt

Auto-assemblage et polymérisation 2D de molécules organiques en surface

Ce travail présente la formation et la caractérisation sous ultravide de monocouches moléculaires issu de l'auto-assemblage et de la polymérisation de molécules organiques (hexahydroxy triphenylène-HHTP et acide diborique benzoïque-BDBA) sur des surfaces monocristallines métalliques et isolantes. L'adsorption de molécules d'HHTP sur Ag(111) donne lieu à plusieurs réseaux moléculaires dépendants de la température. Cette étude, menée par microscopie à effet tunnel (STM), montre qu'un réseau robuste est obtenu suite à la déshydrogénation, activée thermiquement, des groupes alcool périphériques. Cela induit la formation de liaisons hydrogène entre les fonctions alcools et cétones ainsi obtenues. L'étude STM de molécules de BDBA vapo-déposé sur Ag(111) a démontré la formation d'architectures bidimensionnelles étendues, liées de manière covalente, suite à la polymérisation des précurseurs en surface. Un résultat similaire a pu être obtenu par la copolymérisation des molécules de BDBA et d'HHTP. Ces polymères nanoporeux s'étendent en monocouche et présentent une stabilité en température exceptionnelle. Enfin, l'étude de BDBA sur le substrat isolant de KCl(001), menée par microscopie à force atomique en mode non contact (nc-AFM), montre un auto-assemblage étendu par des liaisons hydrogène, et met en évidence le rôle décisif de la nature chimique du substrat sur la faisabilité de la polymérisation de ces molécules en surface. L'approche développée dans ce travail, mettant en jeu des réactions chimiques en surface, constitue une voie nouvelle pour la conception de nano-architectures moléculaires originales et robustes sur surfaces.AIX-MARSEILLE3-BU Sc.St Jérô (130552102) / SudocSudocFranceF