Non-monotonic behavior of the lateral diffusivity in an adsorbate as a function of the surface coverage

Jie Hou; Li Liu; Eugene Mamontov

doi:10.1016/j.commatsci.2019.109299

Non-monotonic behavior of the lateral diffusivity in an adsorbate as a function of the surface coverage

Jie Hou, Li Liu, Eugene Mamontov

Chemical Spectroscopy

Research output: Contribution to journal › Article › peer-review

1 Scopus citations

Abstract

Diffusion dynamics of adsorbate particles confined on a surface strongly depends on the adsorbate surface coverage. Our molecular dynamics simulation reveals that the average lateral diffusivity of the Lennard-Jones adsorbate on a flat substrate varies non-monotonically with the surface coverage. Given that the adsorbate becomes stratified into distinct layers, we propose a novel approach to analyze the lateral diffusion of the adsorbate particles in different layers, via dividing the total lateral diffusion into consecutive lateral diffusion processes, separated by the layer boundary crossing events. A new definition of the lateral diffusivity in the specific layer has been introduced, and it is revealed that the total lateral diffusivity is equal to the sum of lateral diffusivities in different layers. Moreover, the non-monotonic behavior of the average lateral diffusivity with the surface coverage is found to result from the difference in behavior of the lateral diffusivity between the first and other layers.

Original language	English
Article number	109299
Journal	Computational Materials Science
Volume	172
DOIs	https://doi.org/10.1016/j.commatsci.2019.109299
State	Published - Feb 1 2020

Funding

This work was supported as part of the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. Oak Ridge National Laboratory is managed by UT-Battelle, LLC, for U.S. DOE under Contract No. DEAC05-00OR22725. The data required to reproduce these findings are available from the corresponding authors upon reasonable request. This work was supported as part of the Fluid Interface Reactions, Structures and Transport ( FIRST ) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy , Office of Science , Office of Basic Energy Sciences . Oak Ridge National Laboratory is managed by UT- Battelle , LLC, for U.S. DOE under Contract No. DEAC05-00OR22725 .

Funders	Funder number
Energy Frontier Research Center
Office of Basic Energy Sciences
U.S. DOE	DEAC05-00OR22725
UT-Battelle
U.S. Department of Energy
Foundation for Ichthyosis and Related Skin Types
Interface
Office of Science
Oak Ridge National Laboratory

Keywords

Adsorbate
Lateral diffusivity
Lennard-Jones potential
Molecular dynamics
Surface coverage

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10.1016/j.commatsci.2019.109299

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title = "Non-monotonic behavior of the lateral diffusivity in an adsorbate as a function of the surface coverage",

abstract = "Diffusion dynamics of adsorbate particles confined on a surface strongly depends on the adsorbate surface coverage. Our molecular dynamics simulation reveals that the average lateral diffusivity of the Lennard-Jones adsorbate on a flat substrate varies non-monotonically with the surface coverage. Given that the adsorbate becomes stratified into distinct layers, we propose a novel approach to analyze the lateral diffusion of the adsorbate particles in different layers, via dividing the total lateral diffusion into consecutive lateral diffusion processes, separated by the layer boundary crossing events. A new definition of the lateral diffusivity in the specific layer has been introduced, and it is revealed that the total lateral diffusivity is equal to the sum of lateral diffusivities in different layers. Moreover, the non-monotonic behavior of the average lateral diffusivity with the surface coverage is found to result from the difference in behavior of the lateral diffusivity between the first and other layers.",

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AU - Liu, Li

AU - Mamontov, Eugene

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N2 - Diffusion dynamics of adsorbate particles confined on a surface strongly depends on the adsorbate surface coverage. Our molecular dynamics simulation reveals that the average lateral diffusivity of the Lennard-Jones adsorbate on a flat substrate varies non-monotonically with the surface coverage. Given that the adsorbate becomes stratified into distinct layers, we propose a novel approach to analyze the lateral diffusion of the adsorbate particles in different layers, via dividing the total lateral diffusion into consecutive lateral diffusion processes, separated by the layer boundary crossing events. A new definition of the lateral diffusivity in the specific layer has been introduced, and it is revealed that the total lateral diffusivity is equal to the sum of lateral diffusivities in different layers. Moreover, the non-monotonic behavior of the average lateral diffusivity with the surface coverage is found to result from the difference in behavior of the lateral diffusivity between the first and other layers.

AB - Diffusion dynamics of adsorbate particles confined on a surface strongly depends on the adsorbate surface coverage. Our molecular dynamics simulation reveals that the average lateral diffusivity of the Lennard-Jones adsorbate on a flat substrate varies non-monotonically with the surface coverage. Given that the adsorbate becomes stratified into distinct layers, we propose a novel approach to analyze the lateral diffusion of the adsorbate particles in different layers, via dividing the total lateral diffusion into consecutive lateral diffusion processes, separated by the layer boundary crossing events. A new definition of the lateral diffusivity in the specific layer has been introduced, and it is revealed that the total lateral diffusivity is equal to the sum of lateral diffusivities in different layers. Moreover, the non-monotonic behavior of the average lateral diffusivity with the surface coverage is found to result from the difference in behavior of the lateral diffusivity between the first and other layers.

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Non-monotonic behavior of the lateral diffusivity in an adsorbate as a function of the surface coverage

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