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Spectra of the triply charged ion CS[sub 2][sup 3+] and selectivity in molecular Auger effects
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och astronomi, Mjukröntgenfysik.
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2010 (Engelska)Ingår i: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 132, nr 10, s. 104311-Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Spectra of triply charged carbon disulphide have been obtained by measuring, in coincidence, all three electrons ejected in its formation by photoionization. Measurements of the CS23+ ion in coincidence with the three electrons identify the energy range where stable trications are formed. A sharp peak in this energy range is identified as the 2Π ground state at 53.1±0.1 eV, which is the lowest electronic state according to ab initio molecular orbital calculations. Triple ionization by the double Auger effect is provisionally divided, on the basis of the pattern of energy sharing between the two Auger electrons into contributions from direct and cascade Auger processes. The spectra from the direct double Auger effect via S 2p, S 2s, and C 1s hole states contain several resolved features and show selectivity based on the initial charge localization and on the identity of the initial state. Triple ionization spectra from single Auger decay of S 2p -based core-valence states CS22+ show retention of the valence holes in this Auger process. Related ion-electron coincidence measurements give the triple ionization yields and the breakdown patterns in triple photoionization at selected photon energies from 90 eV to above the inner shell edges.

Ort, förlag, år, upplaga, sidor
2010. Vol. 132, nr 10, s. 104311-
Nyckelord [en]
ab initio calculations, Auger effect, carbon compounds, molecule-photon collisions, orbital calculations, photoionisation, positive ions, time of flight spectra
Nationell ämneskategori
Fysik
Identifikatorer
URN: urn:nbn:se:uu:diva-121766DOI: 10.1063/1.3352549ISI: 000275589700025OAI: oai:DiVA.org:uu-121766DiVA, id: diva2:306500
Tillgänglig från: 2010-03-30 Skapad: 2010-03-30 Senast uppdaterad: 2017-12-12Bibliografiskt granskad
Ingår i avhandling
1. Multi-Electron Coincidence Studies of Atoms and Molecules
Öppna denna publikation i ny flik eller fönster >>Multi-Electron Coincidence Studies of Atoms and Molecules
2010 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Abstract [en]

This thesis concerns multi-ionization coincidence measurements of atoms and small molecules using a magnetic bottle time-of-flight (TOF) spectrometer designed for multi-electron coincidence studies. Also, a time-of-flight mass spectrometer has been used together with the TOF electron  spectrometer for electron-ion coincidence measurements. The multi-ionization processes have been studied by employing a pulsed discharge lamp in the vacuum ultraviolet spectral region and synchrotron radiation in the soft X-ray region. The designs of the spectrometers are described in some detail, and several timing schemes suitable for the light sources mentioned above are presented.

Studies have been performed on krypton, molecular oxygen, carbon disulfide and a series of alcohol molecules. For the latter, double ionization spectra have been recorded and new information has been obtained on the dicationic states. A recently found rule-of-thumb  and quantum chemical calculations have been used to quantify the effective distance of the two vacancies in the dications of these molecules.

For Kr, O2, and CS2, single-photon core-valence spectra have been obtained at the synchrotron radiation facility BESSY II in Berlin and interpreted on the basis of quantum chemical calculations. These spectra show a remarkable similarity to conventional valence photoelectron spectra.

Spectra of triply charged ions were recorded, also at BESSY II, for Kr and CS2 by measuring, in coincidence, all three electrons ejected. The complex transition channels leading to tricationic states were mapped in substantial detail for Kr. It was found that for 3d-ionized krypton, the tricationic states are dominantly populated by cascade Auger decays via distinct intermediate states whose energies have been determined. The triple ionization spectra of CS2 from the direct double Auger effect via S2p, S2s and C1s hole states contain several resolved features and show selectivity based on the initial charge localisation and on the identity of the initial state.

Ort, förlag, år, upplaga, sidor
Uppsala: Acta Universitatis Upsaliensis, 2010. s. 71
Serie
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 743
Nyckelord
multi-ionization, electron emission, time-of-flight spectroscopy, coincidence spectroscopy, core-valence ionization, synchrotron radiation, electron correlation
Nationell ämneskategori
Atom- och molekylfysik och optik
Forskningsämne
Fysik med inriktning mot atom- molekyl- och kondenserande materiens fysik
Identifikatorer
urn:nbn:se:uu:diva-122811 (URN)978-91-554-7805-6 (ISBN)
Disputation
2010-05-29, Häggsalen, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 13:15 (Engelska)
Opponent
Handledare
Tillgänglig från: 2010-05-03 Skapad: 2010-04-20 Senast uppdaterad: 2013-09-20

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