Gas-Phase Production of Hydroxylated Silicon Oxide Cluster Cations: Structure, Infrared Spectroscopy, and Astronomical Relevance

The interaction of free cationic silicon oxide clusters, SixOy+ (x = 2–5, y ≥ x), with dilute water vapor, was investigated in a flow tube reactor. Product mass distributions indicate cluster size-dependent dissociative water adsorption. To probe the structure and vibrational spectra of the resultin...

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Authors: Donato, Andreu A. de, Ghejan, Bianca-Andreea, Bakker, Joost M, Bernhardt, Thorsten M., Bromley, Stefan Thomas, Lang, Sandra M.
Format: article
Status:Published version
Publication Date:2024
Country:España
Institution:Universidad de Barcelona
Repository:Dipòsit Digital de la UB
OAI Identifier:oai:dnet:ubarcelona__::71183a9de75f60009ed7f8beedd5e66a
Online Access:https://hdl.handle.net/2445/229521
Access Level:Open access
Keyword:Espectroscòpia infraroja
Compostos de silici
Infrared spectroscopy
Silicon compounds
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spelling Gas-Phase Production of Hydroxylated Silicon Oxide Cluster Cations: Structure, Infrared Spectroscopy, and Astronomical RelevanceDonato, Andreu A. deGhejan, Bianca-AndreeaBakker, Joost MBernhardt, Thorsten M.Bromley, Stefan ThomasLang, Sandra M.Espectroscòpia infrarojaCompostos de siliciInfrared spectroscopySilicon compoundsThe interaction of free cationic silicon oxide clusters, SixOy+ (x = 2–5, y ≥ x), with dilute water vapor, was investigated in a flow tube reactor. Product mass distributions indicate cluster size-dependent dissociative water adsorption. To probe the structure and vibrational spectra of the resulting SixOyH2+ (x = 2–4) clusters, we employed infrared multiple photon dissociation spectroscopy and density functional theory calculations. The planar rhombic cluster core of the disilicon oxides (x = 2) appears to be retained upon dissociative adsorption of one H2O unit, whereas a significant structural transformation of the tri- and tetra-silicon oxides (x = 3 and 4) is induced, resulting in an increased coordination of the Si atoms and more 3D cluster structures. In an astronomical context, we discuss the potential relevance of SixOyHz+ clusters as seeds for dust nucleation and catalysts for carbon-based chemistry in diffuse or translucent interstellar clouds, where all the necessary conditions for producing these species are found. In the produced clusters, the frequency of the isolated silanol Si–OH stretching vibrational mode is considerably blue-shifted compared to that in hydroxylated bulk silica and small inorganic compounds. This mode has a characteristic frequency range between 1200 cm–1 (8.3 μm) and 1090 cm–1 (9.2 μm) and is associated with the anomalously small Si–OH bond lengths in these ionised species. In infrared observations such high frequency Si–O stretching modes are usually associated with a pure bulk silica component of silicate cosmic dust. The presence of SixOyH2+ clusters in low silica astrophysical environments could thus potentially be detected via their signature Si−O band using the James Webb space telescope.American Chemical Society2024info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionapplication/pdfhttps://hdl.handle.net/2445/229521Articles publicats en revistes (Ciència dels Materials i Química Física)reponame:Dipòsit Digital de la UBinstname:Universidad de BarcelonaInglésReproducció del document publicat a: https://doi.org/10.1021/acsearthspacechem.3c00346ACS Earth and Space Chemistry, 2024, vol. 8, num.6, p. 1154-1164https://doi.org/10.1021/acsearthspacechem.3c00346cc by (c) Donato, Andreu A. de et al., 2024https://creativecommons.org/licenses/by/4.0/info:eu-repo/semantics/openAccessoai:dnet:ubarcelona__::71183a9de75f60009ed7f8beedd5e66a2026-05-27T06:46:51Z
dc.title.none.fl_str_mv Gas-Phase Production of Hydroxylated Silicon Oxide Cluster Cations: Structure, Infrared Spectroscopy, and Astronomical Relevance
title Gas-Phase Production of Hydroxylated Silicon Oxide Cluster Cations: Structure, Infrared Spectroscopy, and Astronomical Relevance
spellingShingle Gas-Phase Production of Hydroxylated Silicon Oxide Cluster Cations: Structure, Infrared Spectroscopy, and Astronomical Relevance
Donato, Andreu A. de
Espectroscòpia infraroja
Compostos de silici
Infrared spectroscopy
Silicon compounds
title_short Gas-Phase Production of Hydroxylated Silicon Oxide Cluster Cations: Structure, Infrared Spectroscopy, and Astronomical Relevance
title_full Gas-Phase Production of Hydroxylated Silicon Oxide Cluster Cations: Structure, Infrared Spectroscopy, and Astronomical Relevance
title_fullStr Gas-Phase Production of Hydroxylated Silicon Oxide Cluster Cations: Structure, Infrared Spectroscopy, and Astronomical Relevance
title_full_unstemmed Gas-Phase Production of Hydroxylated Silicon Oxide Cluster Cations: Structure, Infrared Spectroscopy, and Astronomical Relevance
title_sort Gas-Phase Production of Hydroxylated Silicon Oxide Cluster Cations: Structure, Infrared Spectroscopy, and Astronomical Relevance
dc.creator.none.fl_str_mv Donato, Andreu A. de
Ghejan, Bianca-Andreea
Bakker, Joost M
Bernhardt, Thorsten M.
Bromley, Stefan Thomas
Lang, Sandra M.
author Donato, Andreu A. de
author_facet Donato, Andreu A. de
Ghejan, Bianca-Andreea
Bakker, Joost M
Bernhardt, Thorsten M.
Bromley, Stefan Thomas
Lang, Sandra M.
author_role author
author2 Ghejan, Bianca-Andreea
Bakker, Joost M
Bernhardt, Thorsten M.
Bromley, Stefan Thomas
Lang, Sandra M.
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv Espectroscòpia infraroja
Compostos de silici
Infrared spectroscopy
Silicon compounds
topic Espectroscòpia infraroja
Compostos de silici
Infrared spectroscopy
Silicon compounds
description The interaction of free cationic silicon oxide clusters, SixOy+ (x = 2–5, y ≥ x), with dilute water vapor, was investigated in a flow tube reactor. Product mass distributions indicate cluster size-dependent dissociative water adsorption. To probe the structure and vibrational spectra of the resulting SixOyH2+ (x = 2–4) clusters, we employed infrared multiple photon dissociation spectroscopy and density functional theory calculations. The planar rhombic cluster core of the disilicon oxides (x = 2) appears to be retained upon dissociative adsorption of one H2O unit, whereas a significant structural transformation of the tri- and tetra-silicon oxides (x = 3 and 4) is induced, resulting in an increased coordination of the Si atoms and more 3D cluster structures. In an astronomical context, we discuss the potential relevance of SixOyHz+ clusters as seeds for dust nucleation and catalysts for carbon-based chemistry in diffuse or translucent interstellar clouds, where all the necessary conditions for producing these species are found. In the produced clusters, the frequency of the isolated silanol Si–OH stretching vibrational mode is considerably blue-shifted compared to that in hydroxylated bulk silica and small inorganic compounds. This mode has a characteristic frequency range between 1200 cm–1 (8.3 μm) and 1090 cm–1 (9.2 μm) and is associated with the anomalously small Si–OH bond lengths in these ionised species. In infrared observations such high frequency Si–O stretching modes are usually associated with a pure bulk silica component of silicate cosmic dust. The presence of SixOyH2+ clusters in low silica astrophysical environments could thus potentially be detected via their signature Si−O band using the James Webb space telescope.
publishDate 2024
dc.date.none.fl_str_mv 2024
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/2445/229521
url https://hdl.handle.net/2445/229521
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Reproducció del document publicat a: https://doi.org/10.1021/acsearthspacechem.3c00346
ACS Earth and Space Chemistry, 2024, vol. 8, num.6, p. 1154-1164
https://doi.org/10.1021/acsearthspacechem.3c00346
dc.rights.none.fl_str_mv cc by (c) Donato, Andreu A. de et al., 2024
https://creativecommons.org/licenses/by/4.0/
info:eu-repo/semantics/openAccess
rights_invalid_str_mv cc by (c) Donato, Andreu A. de et al., 2024
https://creativecommons.org/licenses/by/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv Articles publicats en revistes (Ciència dels Materials i Química Física)
reponame:Dipòsit Digital de la UB
instname:Universidad de Barcelona
instname_str Universidad de Barcelona
reponame_str Dipòsit Digital de la UB
collection Dipòsit Digital de la UB
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15.811543

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