Shedding Light on the Interfacial Structure of Low-Coverage Alkanethiol Lattices

A comprehensive description of the self-assembly process of alkanethiols on Au(111) is presented, focused on the initial formation of the lying down phases. Low-coverage monolayers are prepared by the disintegration of Au₁₄₄(RS)₆₀ nanoclusters on the reconstructed (22 × √3)-Au(111) surface. The meth...

Descripción completa

Guardado en:
Detalles Bibliográficos
Autores principales: Pensa, Evangelina Laura, Azofra Mesa, Luis Miguel, Albrecht, Tim, Salvarezza, Roberto Carlos, Carro, Pilar
Formato: Articulo
Lenguaje:Inglés
Publicado: 2020
Materias:
Acceso en línea:http://sedici.unlp.edu.ar/handle/10915/123966
Aporte de:
id I19-R120-10915-123966
record_format dspace
institution Universidad Nacional de La Plata
institution_str I-19
repository_str R-120
collection SEDICI (UNLP)
language Inglés
topic Ciencias Exactas
Química
self-assembly process of alkanethiols
alkanethiols
scanning tunneling microscopy
interfacial structure
spellingShingle Ciencias Exactas
Química
self-assembly process of alkanethiols
alkanethiols
scanning tunneling microscopy
interfacial structure
Pensa, Evangelina Laura
Azofra Mesa, Luis Miguel
Albrecht, Tim
Salvarezza, Roberto Carlos
Carro, Pilar
Shedding Light on the Interfacial Structure of Low-Coverage Alkanethiol Lattices
topic_facet Ciencias Exactas
Química
self-assembly process of alkanethiols
alkanethiols
scanning tunneling microscopy
interfacial structure
description A comprehensive description of the self-assembly process of alkanethiols on Au(111) is presented, focused on the initial formation of the lying down phases. Low-coverage monolayers are prepared by the disintegration of Au₁₄₄(RS)₆₀ nanoclusters on the reconstructed (22 × √3)-Au(111) surface. The method provides a limited number of thiols together with a large excess of gold adatoms. Scanning tunneling microscopy and density functional theory calculations were employed to study the transition between low to high thiolate coverage phases. The process involves different lattices and surface transformations, including thiyl radicals on the herringbone reconstruction, radicalinduced herringbone lifting, and the formation of energetically similar metastable phases formed by RS-Au-RS moieties. Results also show that the transition is slow, and different surface structures can coexist on the same sample. Along the process, the first source of Au adatoms to form the RS-Au-SR moieties is the lifting of the herringbone reconstruction because of the lower energetic cost to extract the extra Au atom. However, for hexanethiol (and shorter alkanethiols) at low coverage, additional Au adatoms must be taken from terraces leading to vacancy islands. This process can be entirely suppressed by growing the lying down phases in the presence of an excess of Au adatoms. Taken together, our results shed light on the elusive initial steps of thiol adsorption on clean reconstructed Au, showing that the RS-Au-SR staple motif is also present at the interface of low-coverage self-assembled monolayers.
format Articulo
Articulo
author Pensa, Evangelina Laura
Azofra Mesa, Luis Miguel
Albrecht, Tim
Salvarezza, Roberto Carlos
Carro, Pilar
author_facet Pensa, Evangelina Laura
Azofra Mesa, Luis Miguel
Albrecht, Tim
Salvarezza, Roberto Carlos
Carro, Pilar
author_sort Pensa, Evangelina Laura
title Shedding Light on the Interfacial Structure of Low-Coverage Alkanethiol Lattices
title_short Shedding Light on the Interfacial Structure of Low-Coverage Alkanethiol Lattices
title_full Shedding Light on the Interfacial Structure of Low-Coverage Alkanethiol Lattices
title_fullStr Shedding Light on the Interfacial Structure of Low-Coverage Alkanethiol Lattices
title_full_unstemmed Shedding Light on the Interfacial Structure of Low-Coverage Alkanethiol Lattices
title_sort shedding light on the interfacial structure of low-coverage alkanethiol lattices
publishDate 2020
url http://sedici.unlp.edu.ar/handle/10915/123966
work_keys_str_mv AT pensaevangelinalaura sheddinglightontheinterfacialstructureoflowcoveragealkanethiollattices
AT azoframesaluismiguel sheddinglightontheinterfacialstructureoflowcoveragealkanethiollattices
AT albrechttim sheddinglightontheinterfacialstructureoflowcoveragealkanethiollattices
AT salvarezzarobertocarlos sheddinglightontheinterfacialstructureoflowcoveragealkanethiollattices
AT carropilar sheddinglightontheinterfacialstructureoflowcoveragealkanethiollattices
bdutipo_str Repositorios
_version_ 1764820450584559616