Influence of Molecule–Surface and Molecule–Molecule Interactions on Two-Dimensional Patterns Formed by Functionalized Aromatic Molecules

Fortuna, Sara; Johnston, Karen

doi:10.1021/acs.jpcc.8b01432

Cited by 11 publications

(12 citation statements)

References 34 publications

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“…We start by studying the adsorption of one monolayer of hexachlorobenzene on Pt(111) (see Figure a). This system was selected in the current study since previous experimental work has demonstrated the feasibility of forming a self-assembled monolayer of benzene derivative, including C 6 Cl 6 , on a metal surface. − Theoretically, the Monte Carlo simulations have also predicted that a self-assembled monolayer of hexachlorobenzene (C 6 Cl 6 ) would form at 270 K on the Pt(111) surface. , The adsorption configuration of C 6 Cl 6 adsorbed on the Pt(111) surface, which presents a four-layer slab with the (3 × 3) unit cell, was calculated by the dispersion-inclusive DFT + vdW surf method along with the PBE exchange–correlation functionals. ,− Here, we investigate four high-symmetry adsorption geometries (atop, bridge, fcc, and hcp) with two orientations (0 and 30°) for hexachlorobenzene on the Pt(111) surface. We found that bri30° is the most stable adsorption geometry (see Table S1).…”

Section: Resultsmentioning

confidence: 99%

Conductance Switching in Molecular Self-Assembled Monolayers for Application of Data Storage

Chen

Yang

et al. 2020

J. Phys. Chem. C

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By carrying out dispersion-inclusive density-functional theory computations, we propose a novel type of molecular memory based on the physisorbed and chemisorbed states of a layer of aromatic molecules on metal surfaces. As exemplified by hexachlorobenzene (C6Cl6) on Pt(111), we find that the self-assembled monolayer exhibits an intriguing bistable behavior: molecules can stay stable in either the physiosorbed state (“1”) or the chemisorbed state (“0”), along with a moderate switching barrier. Correspondingly, our transport computations based on the nonequilibrium Green’s function uncover a distinct conductance switching behavior of the molecular layer at the two states. Finally, we determine the thermal stability of the well-defined arrays and demonstrate the feasibility of using a molecule as a bit in an ordered pattern.

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Section: Resultsmentioning

confidence: 99%

Conductance Switching in Molecular Self-Assembled Monolayers for Application of Data Storage

Chen

Yang

et al. 2020

J. Phys. Chem. C

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“…Therefore, many studies apply simplifications at this juncture. For example, they perform Monte Carlo simulations on predefined monomer adsorption grids − or employ machine-learning on coarse-grained models assembled from single-molecule adsorption data. , …”

Section: Introductionmentioning

confidence: 99%

Disordered Two-Dimensional Self-Organization of Ethyl Pyruvate Molecules on the Pt(111) Surface

et al. 2021

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Ethyl pyruvate on a pristine Pt(111) surface in submonolayer coverage neither forms regular superstructures nor a completely random distribution. Instead, a random, widely scattered pattern of a few typical ethyl pyruvate oligomers is found. With global structure optimization of ethyl pyruvate clusters on Pt(111) and without prescribing any adsorption locations or configurations, we can simulate this behavior qualitatively. From an in-depth analysis of our simulation results, we propose that (1) a mix of a large number of possible adsorption configurations leads to disorder, (2) repulsion from molecular charges and dipoles leads to typically large distances between ethyl pyruvate molecules and oligomers, and (3) residual attractive quadrupole interactions lead to remnants of order, in particular to the experimentally observed ethyl pyruvate oligomers with short intraoligomer distances and with typical relative molecular orientations. Additionally, we propose that an experimentally observed, characteristic infrared absorption band for ethyl pyruvate on Pt(111) arises from the surface-perpendicular component of an ester carbonyl vibration directly bound to surface Pt atoms.

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“…One useful method to reduce the experimental efforts mentioned above are the computer simulations in which model parameters can be changed in a quick and easy way . This refers especially to the intrinsic properties of the building block, including its shape, size and distribution of interaction centers.…”

Section: Introductionmentioning

confidence: 99%

“…One useful method to reduce the experimental efforts mentioned above are the computer simulations in which model parameters can be changed in a quick and easy way. [15][16][17][18][19][20][21] This refers especially to the intrinsic properties of the building block, including its shape, size and distribution of interaction centers. Using the simplified coarse grained modeling, these parameters can be readily adjusted to model the 2D self-assembly of a given tecton.…”

Section: Introductionmentioning

confidence: 99%

“…Computer simulations of this type have been successfully used to predict structure formation in adsorbed overlayers comprising different organic molecules. In this field, two main simulation methods can be indicated, that is the Molecular Dynamics (MD) and the Monte Carlo (MC) technique. In the latter case, molecular building blocks have been often represented in a simplified way, so that detailed chemical composition has not been a necessary input and one model structure can refer to a whole class of organic tecons.…”

Section: Introductionmentioning

confidence: 99%

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Surface‐Confined Self‐Assembly of Asymmetric Tetratopic Molecular Building Blocks

Nieckarz

Szabelski

2019

ChemPhysChem

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Surface‐confined self‐assembly of functional molecular building blocks has recently been widely used to create low‐dimensional, also covalent, superstructures with tailorable geometry and physicochemical properties. In this contribution, using the lattice Monte Carlo simulation method, we demonstrate how the structure‐property relation can be established for the 2D self‐assembly of a model tetrapod molecule with reduced symmetry. To that end, a rigid functional unit comprising a few interconnected segments arranged in different tetrapod shapes was used and its self‐assembly on a triangular lattice representing a (111) crystal surface was simulated. The results of our calculations show strong dependence of the structure formation on the molecular symmetry, in particular on the (pro)chiral nature of the building block. The simulations predicted the formation of unusual ordered racemic networks with unique aperiodic spatial distribution of the surface enantiomers. Molecular symmetry was also found to have significant influence on the enantiopure self‐assembly which resulted in the Kagome and brickwall networks and other less ordered extended superstructures with parallelogram pores. The theoretical findings of this contribution can be relevant to designing and on‐surface synthesis of molecular superstructures with predefined geometries and functions. In particular, the predicted molecular architectures can stimulate experimental efforts to fabricate and explore new nanostructures, for example graphitic, having the composition and geometry proposed in our study.

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Influence of Molecule–Surface and Molecule–Molecule Interactions on Two-Dimensional Patterns Formed by Functionalized Aromatic Molecules

Cited by 11 publications

References 34 publications

Conductance Switching in Molecular Self-Assembled Monolayers for Application of Data Storage

Conductance Switching in Molecular Self-Assembled Monolayers for Application of Data Storage

Disordered Two-Dimensional Self-Organization of Ethyl Pyruvate Molecules on the Pt(111) Surface

Surface‐Confined Self‐Assembly of Asymmetric Tetratopic Molecular Building Blocks

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