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Multi-scale Simulation of Equilibrium Step Fluctuations on Cu(111) Surfaces
[Image: see text] Understanding the nature of active sites is a non-trivial task, especially when the catalyst is sensitively affected by chemical reactions and environmental conditions. The challenge lies on capturing explicitly the dynamics of catalyst evolution during reactions. Despite the compl...
Autores principales: | , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2021
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7931195/ https://www.ncbi.nlm.nih.gov/pubmed/33681560 http://dx.doi.org/10.1021/acsomega.0c05064 |
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author | Halim, Harry Handoko Putra, Septia Eka Marsha Muttaqien, Fahdzi Hamada, Ikutaro Inagaki, Kouji Hamamoto, Yuji Morikawa, Yoshitada |
author_facet | Halim, Harry Handoko Putra, Septia Eka Marsha Muttaqien, Fahdzi Hamada, Ikutaro Inagaki, Kouji Hamamoto, Yuji Morikawa, Yoshitada |
author_sort | Halim, Harry Handoko |
collection | PubMed |
description | [Image: see text] Understanding the nature of active sites is a non-trivial task, especially when the catalyst is sensitively affected by chemical reactions and environmental conditions. The challenge lies on capturing explicitly the dynamics of catalyst evolution during reactions. Despite the complexity of catalyst reconstruction, we can untangle them into several elementary processes, of which surface diffusion is of prime importance. By applying density functional theory–kinetic Monte Carlo (DFT–KMC) simulation employed with cluster expansion (CE), we investigated the microscopic mechanism of surface diffusion of Cu with defects such as steps and kinks. Based on the result, the energetics obtained from CE have shown good agreement with DFT calculations. Various diffusion events during the step fluctuations are discussed as well. Aside from the adatom attachment, the diffusion along the step edge is found to be the dominant mass transport mechanism, indicated by the lowest activation energy. We also calculated time correlation functions at 300, 400, and 500 K. However, the time exponent in the correlation function does not strictly follow the power law behavior due to the limited step length, which inhibits variation in the kink density. |
format | Online Article Text |
id | pubmed-7931195 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2021 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-79311952021-03-05 Multi-scale Simulation of Equilibrium Step Fluctuations on Cu(111) Surfaces Halim, Harry Handoko Putra, Septia Eka Marsha Muttaqien, Fahdzi Hamada, Ikutaro Inagaki, Kouji Hamamoto, Yuji Morikawa, Yoshitada ACS Omega [Image: see text] Understanding the nature of active sites is a non-trivial task, especially when the catalyst is sensitively affected by chemical reactions and environmental conditions. The challenge lies on capturing explicitly the dynamics of catalyst evolution during reactions. Despite the complexity of catalyst reconstruction, we can untangle them into several elementary processes, of which surface diffusion is of prime importance. By applying density functional theory–kinetic Monte Carlo (DFT–KMC) simulation employed with cluster expansion (CE), we investigated the microscopic mechanism of surface diffusion of Cu with defects such as steps and kinks. Based on the result, the energetics obtained from CE have shown good agreement with DFT calculations. Various diffusion events during the step fluctuations are discussed as well. Aside from the adatom attachment, the diffusion along the step edge is found to be the dominant mass transport mechanism, indicated by the lowest activation energy. We also calculated time correlation functions at 300, 400, and 500 K. However, the time exponent in the correlation function does not strictly follow the power law behavior due to the limited step length, which inhibits variation in the kink density. American Chemical Society 2021-02-15 /pmc/articles/PMC7931195/ /pubmed/33681560 http://dx.doi.org/10.1021/acsomega.0c05064 Text en © 2021 The Authors. Published by American Chemical Society This is an open access article published under a Creative Commons Attribution (CC-BY) License (http://pubs.acs.org/page/policy/authorchoice_ccby_termsofuse.html) , which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited. |
spellingShingle | Halim, Harry Handoko Putra, Septia Eka Marsha Muttaqien, Fahdzi Hamada, Ikutaro Inagaki, Kouji Hamamoto, Yuji Morikawa, Yoshitada Multi-scale Simulation of Equilibrium Step Fluctuations on Cu(111) Surfaces |
title | Multi-scale Simulation of Equilibrium Step Fluctuations
on Cu(111) Surfaces |
title_full | Multi-scale Simulation of Equilibrium Step Fluctuations
on Cu(111) Surfaces |
title_fullStr | Multi-scale Simulation of Equilibrium Step Fluctuations
on Cu(111) Surfaces |
title_full_unstemmed | Multi-scale Simulation of Equilibrium Step Fluctuations
on Cu(111) Surfaces |
title_short | Multi-scale Simulation of Equilibrium Step Fluctuations
on Cu(111) Surfaces |
title_sort | multi-scale simulation of equilibrium step fluctuations
on cu(111) surfaces |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7931195/ https://www.ncbi.nlm.nih.gov/pubmed/33681560 http://dx.doi.org/10.1021/acsomega.0c05064 |
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