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Opis: The structural patterns formed by molecular self-assembly at surfaces are usually controlled by the relative strengths of the intermolecular and molecule–substrate interactions. An additional steering effect is present when the substrate can easily reconstruct upon molecular adsorption, which therefore drives a self-templating effect on the metal support. This is here demonstrated for the model case of Fe-phthalocyanine molecules adsorbed on the Au(110) surface. Scanning tunneling microscopy shows that molecular adsorption promotes a local (1 × 5) surface reconstruction, which drives the assembly of molecular chains along the [11̅0] direction. The order and periodicity of the molecular assemblies are determined with low energy electron diffraction patterns. Density functional theory calculations reveal the energetic origins of the molecule-driven substrate reconstruction. Since the function of molecular overlayers at surfaces is strongly correlated to their structure, these results have implications in the design of new metal/molecular interfaces.
Najdeno v: ključnih besedah
Povzetek najdenega: ...determined with low energy electron diffraction patterns. Density functional theory calculations reveal the energetic origins...
Ključne besede: self-assembly, phthalocyanine, Au(110), DFT, density functional theory, simulation, surface, recontruction
Objavljeno: 11.10.2016; Ogledov: 3871; Prenosov: 0
Polno besedilo (2,97 MB)

Opis: Iron-phthalocyanine molecules deposited on the Au(110) reconstructed channels assemble into one-dimensional molecular chains, whose spatial distribution evolves into different structural phases at increasing molecular density. The plasticity of the Au channels first induces an ordered phase with a 5×5 symmetry, followed by a second long-range ordered structure composed by denser chains with a 5×7 periodicity with respect to the bare Au surface, as observed in the low-energy electron-diffraction (LEED) and grazing incidence X-ray diffraction (GIXRD) patterns. The geometry of the FePc molecular assemblies in the Au nanorails is determined by scanning tunneling microscopy (STM). For the 5×7 phases, the GIXRD analysis identifies a “4-3” rows profile along the [001] direction in the Au surface and an on-top FePc adsorption site, further confirmed by density functional theory (DFT) calculations. The latter also reveals the electronic mixing of the interface states. The chain assembly is driven by the molecule–molecule interaction and the chains interact with the Au nanorails via the central metal atom, while the chain–chain distance in the different structural phases is primarily driven by the plasticity of the Au surface.
Najdeno v: ključnih besedah
Povzetek najdenega: ...into different structural phases at increasing molecular density. The plasticity of the Au channels first... ...FePc adsorption site, further confirmed by density functional theory (DFT) calculations. The latter also reveals...
Ključne besede: STM, LEED, DFT, density functional theory, phthalocyanine, Au(110), gold, surface
Objavljeno: 13.10.2016; Ogledov: 3944; Prenosov: 0
Polno besedilo (1,33 MB)

Opis: The self-assembly of molecules on surfaces into 2D structures is important for the bottom-up fabrication of functional nanomaterials, and the self-assembledstructure depends on the interplay between molecule-molecule interactions and molecule-surface interactions. Halogenated benzene derivatives on platinum have been shown to have two distinct adsorption states: a physisorbed state and a chemisorbed state, and the interplay between the two can be expected to have a profound effect on the self-assembly and phase behaviour of these systems. We developed a lattice model that explicitly includes both adsorption states, with representative interactions parameterised using density functional theory calculations. This model was used in Monte Carlo simulations to investigate pattern formation of hexahalogenated benzene molecules on the platinumsurface. Molecules that prefer the physisorbed state were found to self-assemble with ease, depending on the interactions between physisorbed molecules. In contrast, molecules that preferentially chemisorb tend to get arrested in disordered phases. However, changing the interactions between chemisorbed and physisorbed molecules affects the phase behaviour. We propose functionalising molecules in order to tune their adsorption states, as an innovative way to control monolayer structure, leading to a promising avenue for directed assembly of novel 2D structures.
Najdeno v: ključnih besedah
Povzetek najdenega: ...adsorption states, with representative interactions parameterised using density functional theory calculations. This model was used...
Ključne besede: lattice model, hexagonal lattice, Monte Carlo, DFT, density functional theory, benzene, physisorption, chemisorption, halogenated
Objavljeno: 11.10.2016; Ogledov: 3737; Prenosov: 0
Polno besedilo (5,75 MB)

Opis: In this work, three surfaces, namely, Mg(0001), Mg(10 ̄1 0) and Mg(11 ̄2 0) are investigated by means of Density Functional Theory and Generalized Gradient Approximation first-principle calculations. The surfaces have been characterized in terms of their interlayer distances, surface energies, Projected Density of States and Surface Core Level Shifts. Contrary to what was found in previous studies based on Density Functional Theory-Local Density Approximation, the use of Generalized Gradient Approximation exchange correlation functional unravels the oscillatory behavior of both interlayer distances and Surface Core Level Shifts of Mg(10 ̄1 0). Moreover, the Projected Density Of States of un-reconstructed Mg(11 ̄2 0) exhibit the typical quantisation of electronic levels associated to a 2D-confinement of a 3D nearly-free electron gas, as observed in nano-wires, and a Peierls instability along the unconfined direction. Different possible reconstructions on Mg(11 ̄2 0) have then been investigated. In particular, it is found that the surface energy of (2X1) and (3X1) reconstructions is almost degenerate and lower than the surface energy of the unreconstructed Mg(11 ̄2 0) surface. Because of the quasi-degeneracy of surface energies, Mg(11 ̄2 0) surface should be composed by a combination of all the quasi degenerate phases.
Najdeno v: ključnih besedah
Povzetek najdenega: ...̄2 0) are investigated by means of Density Functional Theory and Generalized Gradient Approximation first-principle...
Ključne besede: Density Functional Theory, first-principle calculations, Mg surface, Surface Core-Level Shift, surface relaxation, surface reconstruction
Objavljeno: 04.07.2017; Ogledov: 5156; Prenosov: 2086
Polno besedilo (1,77 MB)

Najdeno v: ključnih besedah
Povzetek najdenega: ...features, Rydberg character, Theoretical spectra, Time dependent density functional theory... ...Carbon and nitrogen, General description, Hybrid functional, Near-edge X-ray absorption fine structure spectrum, Relevant...
Ključne besede: Carbon and nitrogen, General description, Hybrid functional, Near-edge X-ray absorption fine structure spectrum, Relevant features, Rydberg character, Theoretical spectra, Time dependent density functional theory
Objavljeno: 19.01.2022; Ogledov: 918; Prenosov: 0
Polno besedilo (4,29 MB)