Free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)m+

Infrared multiple-photon dissociation spectroscopy has been applied to study Ptn(N2O)+ (n = 1–8) clusters which represent entrance-channel complexes on the reactive potential energy surface for nitrous oxide decomposition on platinum. Comparison of spectra recorded in the spectral region 950 cm−1 to...

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Main Authors: Meizyte, G, Green, AE, Gentleman, AS, Schaller, S, Schöllkopf, W, Fielicke, A, Mackenzie, SR
Format: Journal article
Language:English
Published: Royal Society of Chemistry 2020
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author Meizyte, G
Green, AE
Gentleman, AS
Schaller, S
Schöllkopf, W
Fielicke, A
Mackenzie, SR
author_facet Meizyte, G
Green, AE
Gentleman, AS
Schaller, S
Schöllkopf, W
Fielicke, A
Mackenzie, SR
author_sort Meizyte, G
collection OXFORD
description Infrared multiple-photon dissociation spectroscopy has been applied to study Ptn(N2O)+ (n = 1–8) clusters which represent entrance-channel complexes on the reactive potential energy surface for nitrous oxide decomposition on platinum. Comparison of spectra recorded in the spectral region 950 cm−1 to 2400 cm−1 with those simulated for energetically low-lying structures from density functional theory shows a clear preference for molecular binding via the terminal N atom, though evidence of O-binding is observed for some cluster sizes. Enhanced reactivity of Ptn+ n ≥ 6 clusters towards N2O is reflected in the calculated reactive potential energy surfaces and, uniquely in the size range studied, Pt6(N2O)+ proved impossible to form in significant number density even with cryogenic cooling of the cluster source. Infrared-driven N2O decomposition, resulting in the formation of cluster oxides, PtnO+, is observed following vibrational excitation of several Ptn(N2O)+ complexes.
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spelling oxford-uuid:8f4eb5d2-0f50-4f75-aecb-abeb5b8e10152022-03-26T23:03:24ZFree electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)m+Journal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:8f4eb5d2-0f50-4f75-aecb-abeb5b8e1015EnglishSymplectic ElementsRoyal Society of Chemistry2020Meizyte, GGreen, AEGentleman, ASSchaller, SSchöllkopf, WFielicke, AMackenzie, SRInfrared multiple-photon dissociation spectroscopy has been applied to study Ptn(N2O)+ (n = 1–8) clusters which represent entrance-channel complexes on the reactive potential energy surface for nitrous oxide decomposition on platinum. Comparison of spectra recorded in the spectral region 950 cm−1 to 2400 cm−1 with those simulated for energetically low-lying structures from density functional theory shows a clear preference for molecular binding via the terminal N atom, though evidence of O-binding is observed for some cluster sizes. Enhanced reactivity of Ptn+ n ≥ 6 clusters towards N2O is reflected in the calculated reactive potential energy surfaces and, uniquely in the size range studied, Pt6(N2O)+ proved impossible to form in significant number density even with cryogenic cooling of the cluster source. Infrared-driven N2O decomposition, resulting in the formation of cluster oxides, PtnO+, is observed following vibrational excitation of several Ptn(N2O)+ complexes.
spellingShingle Meizyte, G
Green, AE
Gentleman, AS
Schaller, S
Schöllkopf, W
Fielicke, A
Mackenzie, SR
Free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)m+
title Free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)m+
title_full Free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)m+
title_fullStr Free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)m+
title_full_unstemmed Free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)m+
title_short Free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)m+
title_sort free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters ptn n2o m
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