| 1. |
- Gatchell, Michael, et al.
(author)
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First results from the Double ElectroStatic Ion-Ring ExpEriment, DESIREE
- 2014
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In: XXVIII International Conference on Photonic, Electronic and Atomic Collisions (ICPEAC 2013). - : Institute of Physics (IOP). ; 488
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Conference paper (peer-reviewed)abstract
- We have stored the first beams in one of the rings of the double electrostatic ion-storage ring, DESIREE at cryogenic and at room temperature conditions. At cryogenic operations the following parameters are found. Temperature; T= 13K, pressure; p <10(-13) mbar, initial number of stored ions; N > 10(7) and storage lifetime of a C-2(-) beam; tau = 450 S.
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| 2. |
- Gatchell, Michael, et al.
(author)
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Ions colliding with polycyclic aromatic hydrocarbon clusters
- 2013
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In: Physica Scripta. - 0031-8949 .- 1402-4896. ; T156, s. 014062-
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Journal article (peer-reviewed)abstract
- We have measured the ionization and fragmentation of polycyclic aromatic hydrocarbon (PAH) molecules and their clusters. We find that PAH clusters containing up to roughly 100 individual molecules fragment strongly following collisions with keV ions in low or high charge states (q). For both types of collisions, singly charged PAH molecules are found to be the dominant products but for very different reasons. A high-q ion projectile charge leads to strong multiple ionization of the PAH clusters and subsequent Coulomb explosions. A low-q ion projectile charge often leads to single ionization but stronger internal heating and long evaporation sequences with a singly charged PAH monomer as the end product. We have developed a Monte Carlo method for collision-induced heating of PAH clusters and present an evaporation model where the clusters cool slowly as most of the internal energies are stored in intramolecular vibrations and not in molecule-molecule vibrations.
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| 3. |
- Holm, Anne I. S., et al.
(author)
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Ions Colliding with Cold Polycyclic Aromatic Hydrocarbon Clusters
- 2010
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In: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 105:21, s. 213401-
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Journal article (peer-reviewed)abstract
- We report the first experimental study of ions interacting with clusters of polycyclic aromatic hydrocarbon (PAH) molecules. Collisions between 11.25 keV He-3(+) or 360 keV Xe-129(20+) and weakly bound clusters of one of the smallest PAH molecules, anthracene, show that C14H10 clusters have much higher tendencies to fragment in ion collisions than other weakly bound clusters. The ionization is dominated by peripheral collisions in which the clusters, very surprisingly, are more strongly heated by Xe20+ collisions than by He+ collisions. The appearance size is k = 15 for [C14H10](k)(2+).
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| 4. |
- Johansson, Henrik A. B., et al.
(author)
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Ionization and fragmentation of polycyclic aromatic hydrocarbon clusters in collisions with keV ions
- 2011
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In: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 84:4, s. 043201-
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Journal article (peer-reviewed)abstract
- We report on an experimental study of the ionization and fragmentation of clusters of k polycyclic aromatic hydrocarbon (PAH) molecules using anthracene, C14H10, or coronene, C24H12. These PAH clusters are moderately charged and strongly heated in small impact parameter collisions with 22.5-keV He2+ ions, after which they mostly decay in long monomer evaporation sequences with singly charged and comparatively cold monomers as dominating end products. We describe a simple cluster evaporation model and estimate the number of PAH molecules in the clusters that have to be hit by He2+ projectiles for such complete cluster evaporations to occur. Highly charged and initially cold clusters are efficiently formed in collisions with 360-keV Xe20+ ions, leading to cluster Coulomb explosions and several hot charged fragments, which again predominantly yield singly charged, but much hotter, monomer ions than the He2+ collisions. We present a simple formula, based on density-functional-theory calculations, for the ionization energy sequences as functions of coronene cluster size, rationalized in terms of the classic electrostatic expression for the ionization of a charged conducting object. Our analysis indicates that multiple electron removal by highly charged ions from a cluster of PAH molecules rapidly may become more important than single ionization as the cluster size k increases and that this is the main reason for the unexpectedly strong heating in these types of collisions.
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| 5. |
- Lawicki, A., et al.
(author)
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Multiple ionization and fragmentation of isolated pyrene and coronene molecules in collision with ions
- 2011
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In: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 83:2, s. 022704-
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Journal article (peer-reviewed)abstract
- 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.
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| 6. |
- Rousseau, P., et al.
(author)
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Low energy ions interacting with anthracene molecules and clusters
- 2012
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In: Nuclear Instruments and Methods in Physics Research Section B. - : Elsevier BV. - 0168-583X .- 1872-9584. ; 279, s. 140-143
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Journal article (peer-reviewed)abstract
- The interaction of slow ions (nu similar to 0.4 au.) with a small polycyclic aromatic hydrocarbon, namely anthracene (C14H10), is studied in the gas-phase either with the isolated molecule or with a pure cluster target. We discuss the ionization and fragmentation of the molecule with respect to the projectile charge state, i.e. for singly charged He+ ions and for multiply charged Xe20+. ions. For the isolated C14H10, single or multiple ionization of the molecule occurs under ion impact. The (multi) cation relative yields are compared with those obtained by other ionization methods (electron and fs-laser). The molecular dissociation occurs by loss of hydrogen and small hydrocarbon molecules, leading to the formation of CnHx cations. The interaction of Xe20+ with C14H10 clusters gives surprising results, i.e. the emission of hotter monomer compared to the interaction with He+.
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| 7. |
- Seitz, Fabian, et al.
(author)
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Ions colliding with clusters of fullerenes-Decay pathways and covalent bond formations
- 2013
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In: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 139:3
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Journal article (peer-reviewed)abstract
- We report experimental results for the ionization and fragmentation of weakly bound van der Waals clusters of n C-60 molecules following collisions with Ar2+, He2+, and Xe20+ at laboratory kinetic energies of 13 keV, 22.5 keV, and 300 keV, respectively. Intact singly charged C-60 monomers are the dominant reaction products in all three cases and this is accounted for by means of Monte Carlo calculations of energy transfer processes and a simple Arrhenius-type [C-60](n)(+) -> C-60(+) + (n - 1)C-60 evaporation model. Excitation energies in the range of only similar to 0.7 eV per C-60 molecule in a [C-60](13)(+) cluster are sufficient for complete evaporation and such low energies correspond to ion trajectories far outside the clusters. Still we observe singly and even doubly charged intact cluster ions which stem from even more distant collisions. For penetrating collisions the clusters become multiply charged and some of the individual molecules may be promptly fragmented in direct knock-out processes leading to efficient formations of new covalent systems. For Ar2+ and He2+ collisions, we observe very efficient C-119(+) and C-118(+) formation and molecular dynamics simulations suggest that they are covalent dumb-bell systems due to bonding between C-59(+) or C-58(+) and C-60 during cluster fragmentation. In the Ar2+ case, it is possible to form even smaller C-120-2m(+) molecules (m = 2-7), while no molecular fusion reactions are observed for the present Xe20+ collisions.
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| 8. |
- Seitz, Fabian, 1980-
(author)
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Ions colliding with Polycyclic Aromatic Hydrocarbons and Fullerenes
- 2013
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Doctoral thesis (other academic/artistic)abstract
- 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.
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| 9. |
- Seitz, Fabian, 1980-, et al.
(author)
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Polycyclic aromatic hydrocarbon-isomer fragmentation pathways : Case study for pyrene and fluoranthene molecules and clusters
- 2011
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In: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 135:6, s. 064302-
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Journal article (peer-reviewed)abstract
- We report on measurements of the ionization and fragmentation of polycyclic aromatic hydrocarbon (PAH) targets in Xe(20+) + C(16)H(10) and Xe(20+) + [C(16)H(10)](k) collisions and compare results for the two C(16)H(10) isomers: pyrene and fluoranthene. For both types of targets, i.e., for single PAH molecules isolated in vacuum or for isomerically pure clusters of one of the molecules, the resulting fragment spectra are surprisingly similar. However, we do observe weak but significant isomer effects. Although these are manifested in very different ways for the monomer and cluster targets, they both have at their roots small differences (<2.5 eV) between the total binding energies of neutral, and singly and multiply charged pyrene and fluoranthene monomers. The results will be discussed in view of the density functional theory calculations of ionization and dissociation energies for fluoranthene and pyrene. A simple classical over-the-barrier model is used to estimate cross sections for single-and multiple-electron transfer between PAHs and ions. Calculated single and multiple ionization energies, and the corresponding model PAH ionization cross sections, are given.
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| 10. |
- Thomas, Richard D., et al.
(author)
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The double electrostatic ion ring experiment : A unique cryogenic electrostatic storage ring for merged ion-beams studies
- 2011
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In: Review of Scientific Instruments. - : AIP Publishing. - 0034-6748 .- 1089-7623. ; 82:6, s. 065112-
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Journal article (peer-reviewed)abstract
- We describe the design of a novel type of storage device currently under construction at Stockholm University, Sweden, using purely electrostatic focussing and deflection elements, in which ion beams of opposite charges are confined under extreme high vacuum cryogenic conditions in separate rings and merged over a common straight section. The construction of this double electrostatic ion ring experiment uniquely allows for studies of interactions between cations and anions at low and well-defined internal temperatures and centre-of-mass collision energies down to about 10 K and 10 meV, respectively. Position sensitive multi-hit detector systems have been extensively tested and proven to work in cryogenic environments and these will be used to measure correlations between reaction products in, for example, electron-transfer processes. The technical advantages of using purely electrostatic ion storage devices over magnetic ones are many, but the most relevant are: electrostatic elements which are more compact and easier to construct; remanent fields, hysteresis, and eddy-currents, which are of concern in magnetic devices, are no longer relevant; and electrical fields required to control the orbit of the ions are not only much easier to create and control than the corresponding magnetic fields, they also set no upper mass limit on the ions that can be stored. These technical differences are a boon to new areas of fundamental experimental research, not only in atomic and molecular physics but also in the boundaries of these fields with chemistry and biology. For examples, studies of interactions with internally cold molecular ions will be particular useful for applications in astrophysics, while studies of solvated ionic clusters will be of relevance to aeronomy and biology.
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