From a bistable adsorbate to a switchable interface: tetrachloropyrazine on Pt(111)

Hörmann, Lukas; Jeindl, Andreas; Hofmann, Oliver

doi:10.1039/d1nr07763e

Cited by 1 publication

(11 citation statements)

References 52 publications

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“…On the Pt(111) surface, TCP forms chemisorbed and physisorbed adsorption states . In an earlier work, we found strong evidence that chemisorbed TCP forms commensurate and physisorbed TCP forms incommensurate structures. The fact that both systems exhibit both commensurate and incommensurate structures, including static distortion waves in the case of naphthalene on Cu(111), allows us to study the dependence of the frictional properties on static distortion waves.…”

Section: Introductionmentioning

confidence: 53%

“…To determine the energies and forces of all structures [also those of naphthalene on Cu(111)], we use an MLIP. As an improvement over the MLIP used in our previous publication, we now employ a descriptor based on SOAP instead of radial distance functions. For the sake of consistency, we recalculate the formation energy for all structures.…”

Section: Resultsmentioning

confidence: 99%

“…This allows us to produce training data for large unit cells that could not be calculated if the substrate was included. However, the molecule–molecule interaction may be altered significantly due to interactions with the substrate, such as charge transfer or molecular deformations. , This is the case for naphthalene on Cu(111) and chemisorbed TCP on Pt(111), where the interactions change qualitatively. For this reason, it is more accurate to assume noninteracting molecules ( E mol–mol = 0) in the first learning step.…”

Section: Methodsmentioning

confidence: 99%

“…Computational data are reused from previous work: (A) data for naphthalene on Cu(111) come from SAMPLE: surface structure search enabled by coarse-graining and statistical learning and (B) data for TCP on Pt(111) are taken from From a bistable adsorbate to a switchable interface: tetrachloropyrazine on Pt(111). The data are openly available in the NOMAD repository at doi:10.17172/NOMAD/2023.05.01-1 and doi:/10.17172/NOMAD/2022.03.15-1. Information about convergence tests and computational settings can be found in our earlier publications.…”

Section: Methodsmentioning

confidence: 99%

“…Using the Frenkel–Kontorova model, it can be shown that for a surface with a lattice spacing of a and a rigid adsorbate with a lattice spacing of b , lateral forces become infinitesimal beyond a critical value of a / b . However, incommensurate structures are often subject to deformations that may be driven by the forces occurring during interfacial sliding, , or are a result of phase transitions, − or static distortion waves. − The precise quantification of the impact these deformations have on the frictional properties is of great interest for the design of superlubricating interfaces.…”

Section: Introductionmentioning

confidence: 99%

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Impact of Static Distortion Waves on Superlubricity

Hörmann,

Cartus,

Hofmann

2023

ACS Omega

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Friction is a major source of energy loss in mechanical devices. This energy loss may be minimized by creating interfaces with extremely reduced friction, i.e., superlubricity. Conventional wisdom holds that incommensurate interface structures facilitate superlubricity. Accurately describing friction necessitates the precise modeling of the interface structure. This, in turn, requires the use of accurate first-principles electronic structure methods, especially when studying organic/metal interfaces, which are highly relevant due to their tunability and propensity to form incommensurate structures. However, the system size required to calculate incommensurate structures renders such calculations intractable. As a result, studies of incommensurate interfaces have been limited to very simple model systems or strongly simplified methodology. We overcome this limitation by developing a machine-learned interatomic potential that is able to determine energies and forces for structures containing thousands to tens of thousands of atoms with an accuracy comparable to conventional firstprinciples methods but at a fraction of the cost. Using this approach, we quantify the breakdown of superlubricity in incommensurate structures due to the formation of static distortion waves. Moreover, we extract design principles to engineer incommensurate interface systems where the formation of static distortion waves is suppressed, which facilitates low friction coefficients.

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Section: Introductionmentioning

confidence: 53%

Section: Resultsmentioning

confidence: 99%