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Multiple ionization and fragmentation of isolated pyrene and coronene molecules in collision with ions
Stockholms universitet, Naturvetenskapliga fakulteten, Fysikum.
Vise andre og tillknytning
2011 (engelsk)Inngår i: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 83, nr 2, s. 022704-Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

The interaction of multiply charged ions (He2+, O3+, and Xe20+) with gas-phase pericondensed polycyclic aromatic hydrocarbon (PAH) molecules of coronene (C24H12) and pyrene (C16H10) is studied for low-velocity collisions (v <= 0.6 a.u.). The mass spectrometric analysis shows that singly and up to quadruply charged intact molecules are important reaction products. The relative experimental yields are compared with the results of a simple classical over-the-barrier model. For higher molecular charge states, the experimental yields decrease much more strongly than the model predictions due to the instabilities of the multiply charged PAH molecules. Even-odd oscillations with the number of carbon atoms, n, in the intensity distributions of the CnHx+ fragments indicate a linear chain structure of the fragments similar to those observed for ion-C60 collisions. The latter oscillations are known to be due to dissociation energy differences between even-and odd-n Cn-chain molecules. For PAH molecules, the average numbers of H atoms attached to the CnHx chains are larger for even-n reflecting acetylenic bond systems.

sted, utgiver, år, opplag, sider
2011. Vol. 83, nr 2, s. 022704-
HSV kategori
Forskningsprogram
fysik
Identifikatorer
URN: urn:nbn:se:su:diva-63730DOI: 10.1103/PhysRevA.83.022704ISI: 000287076800006OAI: oai:DiVA.org:su-63730DiVA, id: diva2:452021
Tilgjengelig fra: 2011-10-27 Laget: 2011-10-27 Sist oppdatert: 2019-12-04bibliografisk kontrollert
Inngår i avhandling
1. Ionization and Fragmentation of Complex Molecules and Clusters: Biomolecules and Polycyclic Aromatic Hydrocarbons
Åpne denne publikasjonen i ny fane eller vindu >>Ionization and Fragmentation of Complex Molecules and Clusters: Biomolecules and Polycyclic Aromatic Hydrocarbons
2011 (engelsk)Doktoravhandling, med artikler (Annet vitenskapelig)
Abstract [en]

This work deals with ionization and fragmentation of biomolecules and polycyclic aromatic hydrocarbon (PAH) molecules. They are studied in the gas phase both as isolated molecules and as weakly bound clusters. The purpose of the experimental and theoretical investigations are to elucidate charge and energy transfer and related redistribution processes, as well as fragmentation behaviors.

The first part of this thesis presents results from studies on biomolecular ions, in particular nucleotides and peptides, which are primarily examined in electron capture induced dissociation processes. These investigations are relevant for the better understanding of radiation damage to DNA and processes involved in the sequencing of proteins. It is found that the immediate environment have a decisive influence on the fragmentation behaviors. Evaporation of surrounding molecules protect the biomolecules, but their effect on the electronic structure may also enhance or suppress different fragmentation channels.

In the second part of the thesis, results from studies on PAH molecules are presented. Experimentally, their properties are mainly probed through collisions with atomic ion projectiles having kilo-electronvolt kinetic energies. As a widespread pollutant on Earth, and as a family of abundant molecules in space, PAHs are not only relevant from an environmental and health perspective, but they are also important for the understanding of the universe. The present results relate to the stabilities of these molecules, both in isolated form and in clusters, when heated or multiply ionized. It is found to be easier to remove several electrons from clusters of PAH molecules than from isolated PAHs, and fission processes determine their ultimate stabilities. Heated low-charge state clusters of PAHs undergo long evaporation sequences once these have started. For isolated and heated PAHs, internal structural rearrangements are demonstrated to be important in the fragmentation processes.

sted, utgiver, år, opplag, sider
Stockholm: Department of Physics, Stockholm University, 2011. s. 168
HSV kategori
Forskningsprogram
fysik
Identifikatorer
urn:nbn:se:su:diva-63733 (URN)978-91-7447-399-5 (ISBN)
Disputas
2011-12-02, lecture room FB53, AlbaNova universitetscentrum, Roslagstullsbacken 21, Stockholm, 13:00 (engelsk)
Opponent
Veileder
Tilgjengelig fra: 2011-11-10 Laget: 2011-10-27 Sist oppdatert: 2011-11-01bibliografisk kontrollert
2. Ions colliding with Polycyclic Aromatic Hydrocarbons and Fullerenes
Åpne denne publikasjonen i ny fane eller vindu >>Ions colliding with Polycyclic Aromatic Hydrocarbons and Fullerenes
2013 (engelsk)Doktoravhandling, med artikler (Annet vitenskapelig)
Abstract [en]

In this thesis a series of experiments on collisions between atomic projectile ions at keV energies and target vapors of either isolated molecules or van der Waals clusters is presented and analyzed. The atomic ions are produced in an Electron Cyclotron Resonance (ECR) ion source, accelerated and guided into the target volume. The charged target collision products are mass-to-charge analyzed in a time-of-flight spectrometer. The Polycyclic Aromatic Hyrdrocarbons (PAHs) Anthracene (C14H10), Coronene (C24H12), two C16H10 isomers, Pyrene and Fluoranthene, and the fullerene C60 are examined.

For projectile ions in low charge states, small impact parameter collisions dominate, which leads to internal heating of the target. With isolated molecules as targets, this typically results in ionization and often also in fragmentation. For cluster targets energy and charge are rapidly distributed among the cluster building blocks. This is followed by cluster evaporation and very limited fragmentation of the individual molecules. C119+ and C118+ are observed as products. These are due to the formation of the reactive C58/59+ ions by direct knockout processes, which react with another C60 of the cluster to form dumb-bell shaped molecules.

For projectile ions of high charge (Xe20+) larger impact parameters dominate, leading to little internal heating. For isolated molecule targets, intact molecular ions are the main collision products. Charged fragments stem mostly from multifragmentation following ionization to high charge states. For cluster targets, the collision products consist mainly of singly charged monomers. Fragmentation of the individual molecules is comparatively strong. This suggests a quick distribution of charges followed by a Coulomb explosion, which leads to internal heating.

The results show that weakly bound clusters do not sustain the impact of keV-ions and that it is possible to form new molecular structures.

sted, utgiver, år, opplag, sider
Stockholm: Department of Physics, Stockholm University, 2013. s. 118
HSV kategori
Forskningsprogram
fysik
Identifikatorer
urn:nbn:se:su:diva-88427 (URN)978-91-7447-649-1 (ISBN)
Disputas
2013-04-30, lecture hall FD5, AlbaNova universitetscentrum, Roslagstullbacken 21, Stockholm, 10:15 (engelsk)
Opponent
Veileder
Merknad

At the time of doctoral defense, the following papers were unpublished and had a status as follows: Paper 5: Submitted. Paper 6: Submitted.

Tilgjengelig fra: 2013-04-08 Laget: 2013-03-14 Sist oppdatert: 2014-03-28bibliografisk kontrollert

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Holm, Anne I. S.Seitz, FabianJohansson, Henrik A. B.Rosén, StefanSchmidt, Henning T.Zettergren, HenningCederquist, Henrik
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