STM images of multidomain epitaxial graphene on Pt(111) have been combined with a geometrical model to investigate the origin of the coincidence Moiré superstructures. We show that there is a relation between the appearance of a particular Moiré periodicity and the minimization of the absolute value of the strain between the graphene and the substrate for the different orientations between both atomic lattices. This model predicts all the stable epitaxial graphene structures that can be grown on transition metal surfaces, and we have made use of it for reproducing previously published data from different authors. Its validity suggests that minimization of the strain within the coincident graphene unit-cell due to a strong local interaction is the driving force in the formation of Moiré superstructures.
Surface-assisted cyclodehydrogenation and dehydrogenative polymerization of polycyclic (hetero)aromatic hydrocarbons (PAH) are among the most important strategies for bottom-up assembly of new nanostructures from their molecular building blocks. Although diverse compounds have been formed in recent years using this methodology, a limited knowledge on the molecular machinery operating at the nanoscale has prevented a rational control of the reaction outcome. We show that the strength of the PAH-substrate interaction rules the competitive reaction pathways (cyclodehydrogenation versus dehydrogenative polymerization). By controlling the diffusion of N-heteroaromatic precursors, the on-surface dehydrogenation can lead to monomolecular triazafullerenes and diazahexabenzocoronenes (N-doped nanographene), to N-doped oligomeric or polymeric networks, or to carbonaceous monolayers. Governing the on-surface dehydrogenation process is a step forward toward the tailored fabrication of molecular 2D nanoarchitectures distinct from graphene and exhibiting new properties of fundamental and technological interest.
Pinardi, A.L.; Biddau, G.; van de Ruit, K.; Otero-Irurueta, G.; Gardonio, S.; Lizzit, S.; Schennach, R.; Flipse, C.F.J.; Lopez, M.F.; Méndez, J.; Perez, R.; Martin-Gago, J.A. Published in: Nanotechnology DOI:10.1088/0957-4484/25/38/385602Published: 01/01/2014 Document VersionPublisher's PDF, also known as Version of Record (includes final page, issue and volume numbers) Please check the document version of this publication:• A submitted manuscript is the author's version of the article upon submission and before peer-review. There can be important differences between the submitted version and the official published version of record. People interested in the research are advised to contact the author for the final version of the publication, or visit the DOI to the publisher's website.• The final author version and the galley proof are versions of the publication after peer review.• The final published version features the final layout of the paper including the volume, issue and page numbers. Link to publication Citation for published version (APA):Pinardi, A. L., Biddau, G., Ruit, van de, K., Otero-Irurueta, G., Gardonio, S., Lizzit, S., ... Martin-Gago, J. A. (2014). Vacancy formation on C60/Pt (111): unraveling the complex atomistic mechanism. Nanotechnology, 25, 385602-1/13. DOI: 10.1088/0957-4484/25/38/385602 General rightsCopyright and moral rights for the publications made accessible in the public portal are retained by the authors and/or other copyright owners and it is a condition of accessing publications that users recognise and abide by the legal requirements associated with these rights.• Users may download and print one copy of any publication from the public portal for the purpose of private study or research.• You may not further distribute the material or use it for any profit-making activity or commercial gain • You may freely distribute the URL identifying the publication in the public portal ? Take down policyIf you believe that this document breaches copyright please contact us providing details, and we will remove access to the work immediately and investigate your claim. AbstractThe interaction of fullerenes with transition metal surfaces leads to the development of an atomic network of ordered vacancies on the metal. However, the structure and formation mechanism of this intricate surface reconstruction is not yet understood at an atomic level. We combine scanning tunneling microscopy, high resolution and temperature programmed-x-ray photoelectrons spectroscopy, and density functional theory calculations to show that the vacancy formation in C60/Pt(111) is a complex process in which fullerenes undergo two significant structural rearrangements upon thermal annealing. At first, the molecules are physisorbed on the surface; next, they chemisorb inducing the formation of an adatom-vacancy pair on the side of the fullerene. Finally, this metastable state relaxes when the adatom migrates away and the vacancy moves under the molecule. The evolution from a weakly-bound fullerene to a chemisorb...
The intrinsic atomic mechanisms responsible for electronic doping of epitaxial graphene Moirés on transition metal surfaces is still an open issue. To better understand this process we have carried out a first-principles full characterization of the most representative Moiré superstructures observed on the Gr/Pt(111) system and confronted the results with atomically resolved scanning tunneling microscopy experiments. We find that for all reported Moirés the system relaxes inducing a non-negligible atomic corrugation both, at the graphene and at the outermost platinum layer. Interestingly, a mirror “anti-Moiré” reconstruction appears at the substrate, giving rise to the appearance of pinning-points. We show that these points are responsible for the development of the superstructure, while charge from the Pt substrate is injected into the graphene, inducing a local n-doping, mostly localized at these specific pinning-point positions.
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