Interfacial charge rearrangement and intermolecular interactions: Density-functional theory study of free-base porphine adsorbed on Ag(111) and Cu(111)

Müller, Moritz; Diller, Katharina; Maurer, Reinhard J.; Reuter, Karsten

doi:10.1063/1.4938259

Cited by 26 publications

(47 citation statements)

References 57 publications

(84 reference statements)

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“…The lattice parameter of bulk fcc Ag, a = 4.155 Å, calculated using 16×16×16 k-points mesh, was found to agree well with other GGA calculations performed using a similar computational method (e.g. 4.16 Å [ 32 ] or 4.14 Å [ 33 ]) and overestimated the experimental value, 4.086 Å [ 34 ], by less than 1.7%. A silver (111) substrate was modelled with an asymmetric slab consisting of four atomic layers of Ag with a 1×1 or 2×2 surface unit cell.…”

Section: Experimental and Theoretical Methodssupporting

confidence: 77%

On the Structure of Ultrathin FeO Films on Ag(111)

et al. 2018

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Ultrathin transition metal oxide films exhibit unique physical and chemical properties not observed for the corresponding bulk oxides. These properties, originating mainly from the limited thickness and the interaction with the support, make those films similar to other supported 2D materials with bulk counterparts, such as transition metal dichalcogenides. Ultrathin iron oxide (FeO) films, for example, were shown to exhibit unique electronic, catalytic and magnetic properties that depend on the type of the used support. Ag(111) has always been considered a promising substrate for FeO growth, as it has the same surface symmetry, only ~5% lattice mismatch, is considered to be weakly-interacting and relatively resistant to oxidation. The reports on the growth and structure of ultrathin FeO films on Ag(111) are scarce and often contradictory to each other. We attempted to shed more light on this system by growing the films using different preparation procedures and studying their structure using scanning tunneling microscopy (STM), low energy electron diffraction (LEED) and X-ray photoelectron spectroscopy (XPS). We observed the formation of a previously unreported Moiré superstructure with 45 Å periodicity, as well as other reconstructed and reconstruction-free surface species. The experimental results obtained by us and other groups indicate that the structure of FeO films on this particular support critically depends on the films’ preparation conditions. We also performed density functional theory (DFT) calculations on the structure and properties of a conceptual reconstruction-free FeO film on Ag(111). The results indicate that such a film, if successfully grown, should exhibit tunable thickness-dependent properties, being substrate-influenced in the monolayer regime and free-standing-FeO-like when in the bilayer form.

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Section: Experimental and Theoretical Methodssupporting

confidence: 77%

On the Structure of Ultrathin FeO Films on Ag(111)

et al. 2018

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“…This leads to a vacuum layer of around 20 Å between periodic replicas of the system. These values have been proven to be reliable in other similar studies [58]. The bulk cell parameter for silver has the value of 4.08 Å (experimental value).…”

Section: Computational Detailssupporting

confidence: 64%

The effect of translation on the binding energy for transition-metal porphyrines adsorbed on Ag(111) surface

Buimaga-Iarinca

Morari

2019

Beilstein J. Nanotechnol.

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The characteristics of interaction between six transition-metal porphyrines and the Ag(111) surface are detailed here as resulted from DFT calculations. Van der Waals interactions as well as the strong correlation in 3d orbitals of transition metals were taken into account in all calculations, including the structural relaxation. For each system we investigate four relative positions of the metallic atom on top the surface. We show that the interaction between the transition metal and silver is the result of a combination between the dispersion interaction, charge transfer and weak chemical interaction. The detailed analysis of the physical properties, such as dipolar and magnetic moments and the molecule–surface charge transfer, analyzed for different geometric configurations allows us to propose qualitative models, relevant for the understanding of the self-assembly processes and related phenomena.

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“…The van der Waals interaction is taken into account via the optPBE-vdW-DF functional. This ensures that not only directly surface mediated coverage effects are taken into account but also the possible influence of substrate-mediated van der Waals interactions 77 and residual molecule–molecule interactions. From these data, we estimate the coverage correction to beSee the Supporting Information for details on the computational setup and the results.…”

Section: Computational Setupmentioning

confidence: 99%

Quantum Monte Carlo Calculations on a Benchmark Molecule–Metal Surface Reaction: H₂ + Cu(111)

Doblhoff-Dier

Meyer

Hoggan

et al. 2017

J. Chem. Theory Comput.

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Accurate modeling of heterogeneous catalysis requires the availability of highly accurate potential energy surfaces. Within density functional theory, these can—unfortunately—depend heavily on the exchange-correlation functional. High-level ab initio calculations, on the other hand, are challenging due to the system size and the metallic character of the metal slab. Here, we present a quantum Monte Carlo (QMC) study for the benchmark system H2 + Cu(111), focusing on the dissociative chemisorption barrier height. These computationally extremely challenging ab initio calculations agree to within 1.6 ± 1.0 kcal/mol with a chemically accurate semiempirical value. Remaining errors, such as time-step errors and locality errors, are analyzed in detail in order to assess the reliability of the results. The benchmark studies presented here are at the cutting edge of what is computationally feasible at the present time. Illustrating not only the achievable accuracy but also the challenges arising within QMC in such a calculation, our study presents a clear picture of where we stand at the moment and which approaches might allow for even more accurate results in the future.

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Interfacial charge rearrangement and intermolecular interactions: Density-functional theory study of free-base porphine adsorbed on Ag(111) and Cu(111)

Cited by 26 publications

References 57 publications

On the Structure of Ultrathin FeO Films on Ag(111)

On the Structure of Ultrathin FeO Films on Ag(111)

The effect of translation on the binding energy for transition-metal porphyrines adsorbed on Ag(111) surface

Quantum Monte Carlo Calculations on a Benchmark Molecule–Metal Surface Reaction: H₂ + Cu(111)

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Interfacial charge rearrangement and intermolecular interactions: Density-functional theory study of free-base porphine adsorbed on Ag(111) and Cu(111)

Cited by 26 publications

References 57 publications

On the Structure of Ultrathin FeO Films on Ag(111)

On the Structure of Ultrathin FeO Films on Ag(111)

The effect of translation on the binding energy for transition-metal porphyrines adsorbed on Ag(111) surface

Quantum Monte Carlo Calculations on a Benchmark Molecule–Metal Surface Reaction: H2 + Cu(111)

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Quantum Monte Carlo Calculations on a Benchmark Molecule–Metal Surface Reaction: H₂ + Cu(111)