| 1. |
- Gatchell, Michael, et al.
(författare)
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Commissioning of the DESIREE storage rings - a new facility for cold ion-ion collisions
- 2014
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Ingår i: XXVIII International Conference on Photonic, Electronic and Atomic Collisions (ICPEAC 2013). - : Institute of Physics (IOP). ; 488:1
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Konferensbidrag (refereegranskat)abstract
- We report on the ongoing commissioning of the Double ElectroStatic Ion Ring ExpEriment, DESIREE, at Stockholm University. Beams of atomic carbon anions (C-) and smaller carbon anion molecules (C-2(-), C-3(-), C-4(-) etc.) have been produced in a sputter ion source, accelerated to 10 keV or 20 keV, and stored successfully in the two electrostatic rings. The rings are enclosed in a common vacuum chamber cooled to below 13 Kelvin. The DESIREE facility allows for studies of internally relaxed single isolated atomic, molecular and cluster ions and for collision experiments between cat-and anions down to very low center-of-mass collision energies (meV scale). The total thermal load of the vacuum chamber at this temperature is measured to be 32 W. The decay rates of stored ion beams have two components: a non-exponential component caused by the space charge of the beam itself which dominates at early times and an exponential term from the neutralization of the beam in collisions with residual gas at later times. The residual gas limited storage lifetime of carbon anions in the symmetric ring is over seven minutes while the 1/e lifetime in the asymmetric ring is measured to be about 30 seconds. Although we aim to improve the storage in the second ring, the number of stored ions are now sufficient for many merged beams experiments with positive and negative ions requiring milliseconds to seconds ion storage.
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| 2. |
- Chen, Tao, et al.
(författare)
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Absolute fragmentation cross sections in atom-molecule collisions : Scaling laws for non-statistical fragmentation of polycyclic aromatic hydrocarbon molecules
- 2014
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 140:22
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Tidskriftsartikel (refereegranskat)abstract
- We present scaling laws for absolute cross sections for non-statistical fragmentation in collisions between Polycyclic Aromatic Hydrocarbons (PAH/PAH(+)) and hydrogen or helium atoms with kinetic energies ranging from 50 eV to 10 keV. Further, we calculate the total fragmentation cross sections (including statistical fragmentation) for 110 eV PAH/PAH(+) + He collisions, and show that they compare well with experimental results. We demonstrate that non-statistical fragmentation becomes dominant for large PAHs and that it yields highly reactive fragments forming strong covalent bonds with atoms (H and N) and molecules (C6H5). Thus nonstatistical fragmentation may be an effective initial step in the formation of, e. g., Polycyclic Aromatic Nitrogen Heterocycles (PANHs). This relates to recent discussions on the evolution of PAHNs in space and the reactivities of defect graphene structures.
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| 3. |
- da Silva, Humberto, Jr., et al.
(författare)
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Multiple electron capture, excitation, and fragmentation in C6+-C-60 collisions
- 2014
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Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 90:3, s. 032701-
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Tidskriftsartikel (refereegranskat)abstract
- We present experimental and theoretical results on single- and multiple-electron capture, and fragmentation, in C6+ + C-60 collisions at velocities in the v(col) = 0.05 - 0.4 a.u. range. We use time-of-flight mass spectrometry and coincidence detection of charged fragments to separate pure target ionization from processes in which the C-60 target is both ionized and fragmented. The coincidence technique allows us to identify different types of fragmentation processes such as C-60(q+) -> C-58(q+) + C-2 and C-60(q+) -> C-58((q-1)+) + C-2(+). A quasimolecular approach is employed to calculate charge transfer and target excitation cross sections. First-order time-dependent perturbation and statistical methods are used to treat the postcollisional processes: the calculated rate constants for C-2 and C-2(+) emission from the excited and charged fullerene are then used to evaluate the fragmentation dynamics. We show that the target ionization cross section decreases with the induced target charge state and the impact energy. C-2 emission from C-60(q+) is found to dominate when q <= 2 while C-2(+) emission dominates when q >= 5, in agreement with the present and previous experimental results.
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| 4. |
- Gatchell, Michael, et al.
(författare)
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First results from the Double ElectroStatic Ion-Ring ExpEriment, DESIREE
- 2014
-
Ingår i: XXVIII International Conference on Photonic, Electronic and Atomic Collisions (ICPEAC 2013). - : Institute of Physics (IOP). ; 488
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Konferensbidrag (refereegranskat)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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| 5. |
- Gatchell, Michael, et al.
(författare)
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Ions colliding with mixed clusters of C-60 and coronene : Fragmentation and bond formation
- 2014
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Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 90:2
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Tidskriftsartikel (refereegranskat)abstract
- We have studied collisions between 22.5 keV He2+ ions and mixed clusters [(C-60)(m)(C24H12)(n)] of m C-60 and n coronene molecules where m and n range up to about ten. Surprisingly, the cluster fragmentation behavior in distant collisions is dramatically different for pure coronene clusters (m = 0) and clusters containing a single C-60 molecule (m = 1). In the latter case, the clusters may be ionized without also being fragmented on the experimental time scale of tens of microseconds. This does not occur for pure coronene clusters, but is a main characteristic of pure fullerene clusters. For ion trajectories penetrating the mixed cluster, we observe covalent bond formations between C-59 or C-58 and C-60, but not between coronene fragments and C-60, or between C-60 fragments and coronene. These results are explained by means of classical molecular dynamics simulations of collisions inside the fragmenting mixed clusters.
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| 6. |
- Stockett, Mark H., et al.
(författare)
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Fragmentation of anthracene C14H10, acridine C13H9N and phenazine C12H8N2 ions in collisions with atoms
- 2014
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Ingår i: Physical Chemistry, Chemical Physics - PCCP. - : Royal Society of Chemistry (RSC). - 1463-9076 .- 1463-9084. ; 16:40, s. 21980-21987
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Tidskriftsartikel (refereegranskat)abstract
- We report experimental total, absolute, fragmentation cross sections for anthracene C14H10, acridine C13H9N, and phenazine C12H8N2 ions colliding with He at center-of-mass energies close to 100 eV. In addition, we report results for the same ions colliding with Ne, Ar, and Xe at higher energies. The total fragmentation cross sections for these three ions are the same within error bars for a given target. The measured fragment mass distributions reveal significant contributions from both delayed (>> 10(-12) s) statistical fragmentation processes as well as non-statistical, prompt (similar to 10(-15) s), single atom knockout processes. The latter dominate and are often followed by secondary statistical fragmentation. Classical Molecular Dynamics (MD) simulations yield separate cross sections for prompt and delayed fragmentation which are consistent with the experimental results. The intensity of the single C/N-loss peak, the signature of non-statistical fragmentation, decreases with the number of N atoms in the parent ion. The fragment intensity distributions for losses of more than one C or N atom are rather similar for C14H10 and C13H9N but differ strongly for C12H8N2 where weak C-N bonds often remain in the fragments after the first fragmentation step. This greatly increases their probability to fragment further. Distributions of internal energy remaining in the fragments after knockout are obtained from the MD simulations.
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| 7. |
- Stockett, Mark H., et al.
(författare)
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Nonstatistical fragmentation of large molecules
- 2014
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Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 89:3
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Tidskriftsartikel (refereegranskat)abstract
- We present experimental evidence for the dominance of prompt single-atom knockout in fragmenting collisions between large polycyclic aromatic hydrocarbon cations and He atoms at center-of-mass energies close to 100 eV. Such nonstatistical processes are shown to give highly reactive fragments. We argue that nonstatistical fragmentation is dominant for any sufficiently large molecular system under similar conditions.
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| 8. |
- Wang, Y., et al.
(författare)
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Formation dynamics of fullerene dimers C-118(+), C-119(+), and C-120(+)
- 2014
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Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 89:6, s. 062708-
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Tidskriftsartikel (refereegranskat)abstract
- Dumbbell-shaped fullerene dimers C-118(+) and C-119(+) have recently been observed in mass spectra resulting from collisions between clusters of C-60 molecules and keV He2+ or Ar2+ ions [H. Zettergren et al., Phys. Rev. Lett. 110, 185501 (2013) and F. Seitz et al., J. Chem. Phys. 139, 034309 (2013)]. To unveil the formation mechanisms of these fullerene dimers, systematic molecular dynamics (MD) simulations based on the self-consistent charge density functional tight-binding method have been performed for C-n(+) + C-60 (n = 58,59,60) collisions following prompt atom knockouts by the fast ions. The statistics from the MD simulations indicate a much higher reactivity of C-59(+) and C-58(+) fragments compared to that of C-60(+). It is found that the covalently bonded dumbbell-shaped fullerene dimers C-118(+) and C-119(+) can be formed at very low-collision energies within 1 ps and are stable enough to survive on the microsecond time scale of the experiment. The thermodynamic and kinetic stabilities, as well as the bonding features, have been investigated for the most stable dumbbell dimers C-118(+), C-119(+), and C-120(+).
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| 9. |
- Zettergren, Henning, et al.
(författare)
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Bond formation in C-59(+)-C-60 collisions
- 2014
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Ingår i: XXVIII International Conference on Photonic, Electronic and Atomic Collisions (ICPEAC 2013). - : Institute of Physics (IOP).
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Konferensbidrag (refereegranskat)abstract
- In this work, we show that keV-ions are able to remove single carbon atoms from individual fullerenes in clusters of C-60 molecules. This very efficiently leads to the formation of exotic q dumbbell molecules through secondary C-59(+) - C-60 collisions within the fragmenting cluster. Such molecular fusion processes are inherently different from those induced by photons where only products with even numbers of carbon atoms are observed. Thus, ion collisions ignite unique and hitherto overlooked secondary reactions in small aggregates of matter. This relates to the question on how complex molecules may form in e.g. space.
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