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  • 1.
    Amann, Peter
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Degerman, David
    Stockholm University, Faculty of Science, Department of Physics.
    Lee, Ming-Tao
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Shipilin, Mikhail
    Stockholm University, Faculty of Science, Department of Physics.
    Wang, Hsin-Yi
    Stockholm University, Faculty of Science, Department of Physics.
    Cavalca, Filippo
    Weston, Matthew
    Stockholm University, Faculty of Science, Department of Physics.
    Gladh, Jörgen
    Stockholm University, Faculty of Science, Department of Physics.
    Blom, Mikael
    Stockholm University, Faculty of Science, Department of Physics.
    Björkhage, Mikael
    Stockholm University, Faculty of Science, Department of Physics.
    Löfgren, Patrik
    Stockholm University, Faculty of Science, Department of Physics.
    Schlueter, Christoph
    Drube, Wofgang
    Lömker, Patrick
    Ederer, Katrin
    Noei, Heshmat
    Zehetner, Johann
    Wentzel, Henrik
    Åhlund, John
    Nilsson, Anders
    Stockholm University, Faculty of Science, Department of Physics.
    A dedicated photoelectron spectroscopy instrument for studies of catalytic reactions at pressures exceeding 1 barManuscript (preprint) (Other academic)
    Abstract [en]

    Here, we present a new high-pressure x-ray photoelectron spectroscopy system dedicated to probing catalytic reactions under realistic conditions at pressures exceeding 1 bar. The instrument builds around the concept of a “virtual cell” in which a gasflow is directed onto the sample surface creating a local high pressure on top of the sample. This allows the instrument to maintain a low pressure of a few mbars in the main chamber, while simultaneously keeping a local pressure of around 1 bar. Synchrotron radiation based grazing incidence photoemission within ± 5° is used to enhance the surface sensitivity in the experiment. The aperture, separating the high-pressure region from the differential pumping of the electron spectrometer, consists of multiple, evenly spaced, mm sized holes matching the footprint of the x-ray beam on the sample surface. As the photo-emitted electrons are subject to strong scattering in the gas phase and the resulting signal is therefore highly dependent on the sample to aperture distance, the latter is controlled with high precision using a fully integrated manipulator that allows for sample movement with step sizes of 10 nm between 0 and –5 mm with very low vibrational amplitude. The instrumental features allows acquisition of metallic bulk spectra at He pressures up to 2.5 bar and also allows for following C1s spectra under realistic gas mixtures of CO + H2with various temperatures up to 500°C. This capability opens for studies of catalytic reactions in operandi.

  • 2.
    Amann, Peter
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Degerman, David
    Stockholm University, Faculty of Science, Department of Physics.
    Lee, Ming-Tao
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Shipilin, Mikhail
    Stockholm University, Faculty of Science, Department of Physics.
    Wang, Hsin-Yi
    Stockholm University, Faculty of Science, Department of Physics.
    Cavalca, Filippo
    Stockholm University, Faculty of Science, Department of Physics.
    Weston, Matthew
    Stockholm University, Faculty of Science, Department of Physics.
    Gladh, Jörgen
    Stockholm University, Faculty of Science, Department of Physics.
    Blom, Mikael
    Stockholm University, Faculty of Science, Department of Physics.
    Björkhage, Mikael
    Stockholm University, Faculty of Science, Department of Physics.
    Löfgren, Patrik
    Stockholm University, Faculty of Science, Department of Physics.
    Schlueter, Christoph
    Loemker, Patrick
    Ederer, Katrin
    Drube, Wolfgang
    Noei, Heshmat
    Zehetner, Johann
    Wentzel, Henrik
    Ahlund, John
    Nilsson, Anders
    Stockholm University, Faculty of Science, Department of Physics.
    A high-pressure x-ray photoelectron spectroscopy instrument for studies of industrially relevant catalytic reactions at pressures of several bars2019In: Review of Scientific Instruments, ISSN 0034-6748, E-ISSN 1089-7623, Vol. 90, no 10, article id 103102Article in journal (Refereed)
    Abstract [en]

    We present a new high-pressure x-ray photoelectron spectroscopy system dedicated to probing catalytic reactions under realistic conditions at pressures of multiple bars. The instrument builds around the novel concept of a virtual cell in which a gas flow onto the sample surface creates a localized high-pressure pillow. This allows the instrument to be operated with a low pressure of a few millibar in the main chamber, while simultaneously a local pressure exceeding 1 bar can be supplied at the sample surface. Synchrotron based hard x-ray excitation is used to increase the electron mean free path in the gas region between sample and analyzer while grazing incidence <5 degrees close to total external refection conditions enhances surface sensitivity. The aperture separating the high-pressure region from the differential pumping of the electron spectrometer consists of multiple, evenly spaced, micrometer sized holes matching the footprint of the x-ray beam on the sample. The resulting signal is highly dependent on the sample-to-aperture distance because photoemitted electrons are subject to strong scattering in the gas phase. Therefore, high precision control of the sample-to-aperture distance is crucial. A fully integrated manipulator allows for sample movement with step sizes of 10 nm between 0 and -5 mm with very low vibrational amplitude and also for sample heating up to 500 degrees C under reaction conditions. We demonstrate the performance of this novel instrument with bulk 2p spectra of a copper single crystal at He pressures of up to 2.5 bars and C1s spectra measured in gas mixtures of CO + H-2 at pressures of up to 790 mbar. The capability to detect emitted photoelectrons at several bars opens the prospect for studies of catalytic reactions under industrially relevant operando conditions.

  • 3.
    Chen, Tao
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Forsberg, Björn
    Stockholm University, Faculty of Science, Department of Physics.
    Pettersson, Alf
    Stockholm University, Faculty of Science, Department of Physics.
    Gatchell, Michael
    Stockholm University, Faculty of Science, Department of Physics.
    Cederquist, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    Zettergren, Henning
    Stockholm University, Faculty of Science, Department of Physics.
    Modeling electron and energy transfer processes in collisions between ions and Polycyclic Aromatic Hydrocarbon molecules2014In: 17th International Conference on Calorimetry in Particle Physics (CALOR2016), 2014, article id 102015Conference paper (Refereed)
    Abstract [en]

    In this work we study collisions between ions and Polycyclic Aromatic Hydrocarbons with the aid of a novel over-the-barrier model and well-established models for nuclear and electronic stopping processes.

  • 4.
    Chen, Tao
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Gatchell, Michael
    Stockholm University, Faculty of Science, Department of Physics.
    Stockett, Mark H.
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Zhang, Y.
    Rousseau, P.
    Domaracka, A.
    Maclot, S.
    Delaunay, R.
    Adoui, L.
    Huber, B. A.
    Schlatholter, T.
    Schmidt, Henning T.
    Stockholm University, Faculty of Science, Department of Physics.
    Cederquist, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    Zettergren, Henning
    Stockholm University, Faculty of Science, Department of Physics.
    Absolute fragmentation cross sections in atom-molecule collisions: Scaling laws for non-statistical fragmentation of polycyclic aromatic hydrocarbon molecules2014In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 140, no 22, article id 224306Article in journal (Refereed)
    Abstract [en]

    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.

  • 5.
    de Ruette, Nathalie
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Wolf, Michael
    Stockholm University, Faculty of Science, Department of Physics.
    Giacomozzi, Linda
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Gatchell, Michael
    Stockholm University, Faculty of Science, Department of Physics. Universität Innsbruck, Austria.
    Stockett, Mark H.
    Stockholm University, Faculty of Science, Department of Physics.
    Haag, Nicole
    Stockholm University, Faculty of Science, Department of Physics.
    Zettergren, Henning
    Stockholm University, Faculty of Science, Department of Physics.
    Schmidt, Henning T.
    Stockholm University, Faculty of Science, Department of Physics.
    Cederquist, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    DESIREE electrospray ion source test bench and setup for collision induced dissociation experiments2018In: Review of Scientific Instruments, ISSN 0034-6748, E-ISSN 1089-7623, Vol. 89, no 7, article id 075102Article in journal (Refereed)
    Abstract [en]

    In this paper, we give a detailed description of an electrospray ion source test bench and a single-pass setup for ion fragmentation studies at the Double ElectroStatic Ion Ring ExpEriment infrastructure at Stockholm University. This arrangement allows for collision-induced dissociation experiments at the center-of-mass energies between 10 eV and 1 keV. Charged fragments are analyzed with respect to their kinetic energies (masses) by means of an electrostatic energy analyzer with a wide angular acceptance and adjustable energy resolution.

  • 6.
    Forsberg, B. O.
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Chen, Tao
    Stockholm University, Faculty of Science, Department of Physics.
    Pettersson, A. T.
    Stockholm University, Faculty of Science, Department of Physics.
    Gatchell, Michael
    Stockholm University, Faculty of Science, Department of Physics.
    Cederquist, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    Zettergren, Henning
    Stockholm University, Faculty of Science, Department of Physics.
    Ions interacting with planar aromatic molecules: Modeling electron transfer reactions2013In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 138, no 5, p. 054306-Article in journal (Refereed)
    Abstract [en]

    We present theoretical absolute charge exchange cross sections for multiply charged cations interacting with the Polycyclic Aromatic Hydrocarbon (PAH) molecules pyrene C14H10, coronene C24H12, or circumcoronene C54H18. These planar, nearly circular, PAHs are modelled as conducting, infinitely thin, and perfectly circular discs, which are randomly oriented with respect to straight line ion trajectories. We present the analytical solution for the potential energy surface experienced by an electron in the field of such a charged disc and a point-charge at an arbitrary position. The location and height of the corresponding potential energy barrier from this simple model are in close agreement with those from much more computationally demanding Density Functional Theory (DFT) calculations in a number of test cases. The model results compare favourably with available experimental data on single-and multiple electron transfer reactions and we demonstrate that it is important to include the orientation dependent polarizabilities of the molecules (model discs) in particular for the larger PAHs. PAH ionization energy sequences from DFT are tabulated and used as model inputs. Absolute cross sections for the ionization of PAH molecules, and PAH ionization energies such as the ones presented here may be useful when considering the roles of PAHs and their ions in, e. g., interstellar chemistry, stellar atmospheres, and in related photoabsorption and photoemission spectroscopies.

  • 7.
    Gatchell, Michael
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Schmidt, Henning T.
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Andler, Guillermo
    Stockholm University, Faculty of Science, Department of Physics.
    Björkhage, Mikael
    Stockholm University, Faculty of Science, Department of Physics.
    Blom, Mikael
    Stockholm University, Faculty of Science, Department of Physics.
    Brännholm, Lars
    Stockholm University, Faculty of Science, Department of Physics.
    Bäckström, Erik
    Stockholm University, Faculty of Science, Department of Physics.
    Chen, Tao
    Stockholm University, Faculty of Science, Department of Physics.
    Geppert, Wolf
    Stockholm University, Faculty of Science, Department of Physics.
    Halldén, Per
    Stockholm University, Faculty of Science, Department of Physics.
    Hanstorp, Dag
    Hellberg, Fredrik
    Stockholm University, Faculty of Science, Department of Physics.
    Källberg, Anders
    Stockholm University, Faculty of Science, Department of Physics.
    Larsson, Mats
    Stockholm University, Faculty of Science, Department of Physics.
    Leontein, Sven
    Stockholm University, Faculty of Science, Department of Physics.
    Liljeby, Leif
    Stockholm University, Faculty of Science, Department of Physics.
    Löfgren, Patrik
    Stockholm University, Faculty of Science, Department of Physics.
    Mannervik, Sven
    Stockholm University, Faculty of Science, Department of Physics.
    Paal, Andras
    Stockholm University, Faculty of Science, Department of Physics.
    Reinhed, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Rensfelt, Karl-Gunnar
    Stockholm University, Faculty of Science, Department of Physics.
    Rosén, Stefan
    Stockholm University, Faculty of Science, Department of Physics.
    Seitz, Fabian
    Stockholm University, Faculty of Science, Department of Physics.
    Simonsson, Ansgar
    Stockholm University, Faculty of Science, Department of Physics.
    Stockett, Mark H.
    Stockholm University, Faculty of Science, Department of Physics.
    Thomas, Richard D.
    Stockholm University, Faculty of Science, Department of Physics.
    Zettergren, Henning
    Stockholm University, Faculty of Science, Department of Physics.
    Cederquist, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    First results from the Double ElectroStatic Ion-Ring ExpEriment, DESIREE2014In: XXVIII International Conference on Photonic, Electronic and Atomic Collisions (ICPEAC 2013), Institute of Physics (IOP), 2014, article id 092003Conference paper (Refereed)
    Abstract [en]

    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.

  • 8.
    Gatchell, Michael
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Schmidt, Henning T.
    Stockholm University, Faculty of Science, Department of Physics.
    Thomas, Richard D.
    Stockholm University, Faculty of Science, Department of Physics.
    Rosén, Stefan
    Stockholm University, Faculty of Science, Department of Physics.
    Reinhed, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Löfgren, Patrik
    Stockholm University, Faculty of Science, Department of Physics.
    Brännholm, Lars
    Stockholm University, Faculty of Science, Department of Physics.
    Blom, Mikael
    Stockholm University, Faculty of Science, Department of Physics.
    Björkhage, Mikael
    Stockholm University, Faculty of Science, Department of Physics.
    Bäckström, Erik
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Leontein, Sven
    Stockholm University, Faculty of Science, Department of Physics.
    Hanstorp, D.
    Zettergren, Henning
    Stockholm University, Faculty of Science, Department of Physics.
    Liljeby, Leif
    Stockholm University, Faculty of Science, Department of Physics.
    Källberg, Anders
    Stockholm University, Faculty of Science, Department of Physics.
    Simonsson, Ansgar
    Stockholm University, Faculty of Science, Department of Physics.
    Hellberg, Fredrik
    Stockholm University, Faculty of Science, Department of Physics.
    Mannervik, Sven
    Stockholm University, Faculty of Science, Department of Physics.
    Larsson, Mats
    Stockholm University, Faculty of Science, Department of Physics.
    Geppert, Wolf D.
    Stockholm University, Faculty of Science, Department of Physics.
    Rensfelt, Karl-Gunnar
    Stockholm University, Faculty of Science, Department of Physics.
    Danared, Håkan
    Stockholm University, Faculty of Science, Department of Physics. European Spallation Source, Sweden.
    Paál, Andras
    Stockholm University, Faculty of Science, Department of Physics.
    Masuda, Masaharu
    Stockholm University, Faculty of Science, Department of Physics.
    Halldén, Per
    Stockholm University, Faculty of Science, Department of Physics.
    Andler, Guillermo
    Stockholm University, Faculty of Science, Department of Physics.
    Stockett, Mark H.
    Stockholm University, Faculty of Science, Department of Physics.
    Chen, Tao
    Stockholm University, Faculty of Science, Department of Physics.
    Källersjö, Gunnar
    Stockholm University, Faculty of Science, Department of Physics.
    Weimer, Jan
    Stockholm University, Faculty of Science, Department of Physics.
    Hansen, K.
    Hartman, H.
    Cederquist, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    Commissioning of the DESIREE storage rings - a new facility for cold ion-ion collisions2014In: XXVIII International Conference on Photonic, Electronic and Atomic Collisions (ICPEAC 2013), Institute of Physics (IOP), 2014, article id 012040Conference paper (Refereed)
    Abstract [en]

    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.

  • 9.
    Gatchell, Michael
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Zettergren, Henning
    Stockholm University, Faculty of Science, Department of Physics.
    Seitz, Fabian
    Stockholm University, Faculty of Science, Department of Physics.
    Chen, Tao
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Stocket, Mark H.
    Stockholm University, Faculty of Science, Department of Physics.
    Schmidt, Henning T.
    Stockholm University, Faculty of Science, Department of Physics.
    Lawicki, A.
    Rangama, J.
    Rousseau, P.
    Capron, M.
    Maclot, S.
    Maisonny, R.
    Domaracka, A.
    Adoui, L.
    Mery, A.
    Chesnel, J-Y
    Manil, B.
    Huber, B. A.
    Cederquist, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    Ions colliding with polycyclic aromatic hydrocarbon clusters2013In: Physica Scripta, ISSN 0031-8949, E-ISSN 1402-4896, Vol. T156, p. 014062-Article in journal (Refereed)
    Abstract [en]

    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.

  • 10.
    Kulyk, Kostiantyn
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Borysenko, Mykola
    Kulik, Tetiana
    Mikhalovska, Lyuba
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Palianytsia, Borys
    Chemisorption and thermally induced transformations of polydimethylsiloxane on the surface of nanoscale silica and ceria/silica2015In: Polymer degradation and stability, ISSN 0141-3910, E-ISSN 1873-2321, Vol. 120, p. 203-211Article in journal (Refereed)
    Abstract [en]

    Compositions of polydimethylsiloxane (PDMS) polymer with nanosized silica and ceria/silica were prepared. The influence of these nano-fillers on the thermal stability and degradation mechanism of silicone polymer was investigated using Thermogravimetric Analysis (TGA) and Temperature Programmed Desorption Mass Spectrometry (TPD MS). The results showed that thermal decomposition of pure and adsorbed PDMS differs significantly. The three main stages of the PDMS thermal transformations in the adsorbed state were determined to be: 1) chemisorption of PDMS chains involving the terminal trimethylsilyl groups of the polymer and silanol groups of the silica surface; 2) formation and desorption of cyclic oligomers; 3) high temperature radical degradation of the polymer accompanied by the formation of methane and ethylene. The kinetic parameters of the corresponding reactions were calculated from the TPD MS data. It was found that nanoparticles of cerium dioxide strongly influence the degradation pattern, lower the decomposition temperature and catalyze the formation of methane.

  • 11.
    Kulyk, Kostiantyn
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Palianytsia, Borys
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Azizova, Liana
    Borysenko, Mykola
    Kartel, Mykola
    Larsson, Mats
    Stockholm University, Faculty of Science, Department of Physics.
    Kulik, Tetiana
    Kinetics of Valeric Acid Ketonization and Ketenization in Catalytic Pyrolysis on Nanosized SiO2, gamma-Al2O3, CeO2/SiO2, Al2O3/SiO2 and TiO2/SiO22017In: ChemPhysChem, ISSN 1439-4235, E-ISSN 1439-7641, Vol. 18, no 14, p. 1943-1955Article in journal (Refereed)
    Abstract [en]

    Valeric acid is an important renewable platform chemical that can be produced efficiently from lignocellulosic biomass. Upgrading of valeric acid by catalytic pyrolysis has the potential to produce value added biofuels and chemicals on an industrial scale. Understanding the different mechanisms involved in the thermal transformations of valeric acid on the surface of nanometer-sized oxides is important for the development of efficient heterogeneously catalyzed pyrolytic conversion techniques. In this work, the thermal decomposition of valeric acid on the surface of nanoscale SiO2, gamma-Al2O3, CeO2/SiO2, Al2O3/SiO2 and TiO2/SiO2 has been investigated by temperature-programmed desorption mass spectrometry (TPD MS). Fourier transform infrared spectroscopy (FTIR) has also been used to investigate the structure of valeric acid complexes on the oxide surfaces. Two main products of pyrolytic conversion were observed to be formed depending on the nano-catalyst used-dibutylketone and propylketene. Mechanisms of ketene and ketone formation from chemisorbed fragments of valeric acid are proposed and the kinetic parameters of the corresponding reactions were calculated. It was found that the activation energy of ketenization decreases in the order SiO2 > gamma-Al2O3 > TiO2/SiO2 > Al2O3/SiO2, and the activation energy of ketonization decreases in the order gamma-Al2O3 > CeO2/SiO2. Nanooxide CeO2/SiO2 was found to selectively catalyze the ketonization reaction.

  • 12.
    Kulyk, Kostiantyn
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Rebrov, Oleksii
    Stockholm University, Faculty of Science, Department of Physics.
    Stockett, Mark H.
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Zettergren, Henning
    Stockholm University, Faculty of Science, Department of Physics.
    Schmidt, Henning T.
    Stockholm University, Faculty of Science, Department of Physics.
    Thomas, Richard D.
    Stockholm University, Faculty of Science, Department of Physics.
    Cederquist, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    Larsson, Mats
    Stockholm University, Faculty of Science, Department of Physics.
    High-energy collisions of protonated enantiopure amino acids with a chiral target gas2015In: International Journal of Mass Spectrometry, ISSN 1387-3806, E-ISSN 1873-2798, Vol. 388, p. 59-64Article in journal (Refereed)
    Abstract [en]

    We have studied the fragmentation of the singly protonated L- and D-forms of enantiomerically pure phenylalanine (Phe), tryptophan (Trp), and methionine (Met) in high-energy collisions with chiral and achiral gas targets. (S)-(+)-2-butanol, racemic (+/-)-2-butanol, and argon were used as target gases. At center-of-mass frame collision energy of I key, it was found that all of the ions exhibit common fragmentation pathways which are independent of target chirality. For all projectile ions, the elimination of NH3 and H2O + CO were found to be the main reaction channels. The observed fragmentation patterns were dominated by statistically driven processes. The energy deposited into the ions was found to be sufficient to yield multiple fragment ions, which arise from decomposition via various competitive reaction pathways.

  • 13.
    Kulyk, Kostiantyn
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Zettergren, Henning
    Stockholm University, Faculty of Science, Department of Physics.
    Gatchell, Michael
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Borysenko, Mykola
    Palianytsia, Borys
    Larsson, Mats
    Stockholm University, Faculty of Science, Department of Physics.
    Kulik, Tetiana
    Dimethylsilanone Generation from Pyrolysis of Polysiloxanes Filled with Nanosized Silica and Ceria/Silica2016In: chempluschem, ISSN 2192-6506, Vol. 81, no 9, p. 1003-1013Article in journal (Refereed)
    Abstract [en]

    Temperature-programmed desorption mass spectrometry (TPDMS) was used to study the pyrolysis of PDMS and its composites with nanosized silica and ceria/silica. The results suggest that the elusive organosilicon compound, dimethylsilanone, is generated from PDMS over a broad temperature range (in some cases starting at 70 degrees C). The presence of nano-oxides catalyzes this process. Ions characteristic of the fragmentation of dimethylsilanone under electron ionization are assigned with the aid of DFT structure calculations. Possible reaction mechanisms for dimethylsilanone generation are discussed in the context of the calculated kinetic parameters. Observed accompanying products of PDMS pyrolysis, such as tetramethylcyclodisiloxane and hexamethylcyclotrisiloxane, indicate that multiple channels are involved in the dimethylsilanone release.

  • 14.
    Schmidt, Henning T.
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Thomas, Richard D.
    Stockholm University, Faculty of Science, Department of Physics.
    Gatchell, Michael
    Stockholm University, Faculty of Science, Department of Physics.
    Rosén, Stefan
    Stockholm University, Faculty of Science, Department of Physics.
    Reinhed, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Löfgren, Patrik
    Stockholm University, Faculty of Science, Department of Physics.
    Brännholm, Lars
    Stockholm University, Faculty of Science, Department of Physics.
    Blom, Mikael
    Stockholm University, Faculty of Science, Department of Physics.
    Björkhage, Mikael
    Stockholm University, Faculty of Science, Department of Physics.
    Bäckström, Erik
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Leontein, Sven
    Stockholm University, Faculty of Science, Department of Physics.
    Hanstorp, D.
    Zettergren, Henning
    Stockholm University, Faculty of Science, Department of Physics.
    Liljeby, Leif
    Stockholm University, Faculty of Science, Department of Physics.
    Källberg, Anders
    Stockholm University, Faculty of Science, Department of Physics.
    Simonsson, Ansgar
    Stockholm University, Faculty of Science, Department of Physics.
    Hellberg, Fredrik
    Stockholm University, Faculty of Science, Department of Physics.
    Mannervik, Sven
    Stockholm University, Faculty of Science, Department of Physics.
    Larsson, Mats
    Stockholm University, Faculty of Science, Department of Physics.
    Geppert, Wolf D.
    Stockholm University, Faculty of Science, Department of Physics.
    Rensfelt, Karl-Gunnar
    Stockholm University, Faculty of Science, Department of Physics.
    Danared, Håkan
    Stockholm University, Faculty of Science, Department of Physics.
    Paal, A.
    Stockholm University, Faculty of Science, Department of Physics.
    Masuda, Masaharu
    Stockholm University, Faculty of Science, Department of Physics.
    Hallden, Per
    Stockholm University, Faculty of Science, Department of Physics.
    Andler, Guillermo
    Stockholm University, Faculty of Science, Department of Physics.
    Stockett, Mark H.
    Stockholm University, Faculty of Science, Department of Physics.
    Chen, Tao
    Stockholm University, Faculty of Science, Department of Physics.
    Källersjö, Gunnar
    Stockholm University, Faculty of Science, Department of Physics.
    Weimer, Jan
    Stockholm University, Faculty of Science, Department of Physics.
    Hansen, K.
    Hartman, H.
    Cederquist, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    First storage of ion beams in the Double Electrostatic Ion-Ring Experiment: DESIREE2013In: Review of Scientific Instruments, ISSN 0034-6748, E-ISSN 1089-7623, Vol. 84, no 5, p. 055115-Article in journal (Refereed)
    Abstract [en]

    We report on the first storage of ion beams in the Double ElectroStatic Ion Ring ExpEriment, DESIREE, at Stockholm University. We have produced beams of atomic carbon anions and small carbon anion molecules (C-n(-), n = 1, 2, 3, 4) in a sputter ion source. The ion beams were accelerated to 10 keV kinetic energy and stored in an electrostatic ion storage ring enclosed in a vacuum chamber at 13 K. For 10 keV C-2(-) molecular anions we measure the residual-gas limited beam storage lifetime to be 448 s +/- 18 s with two independent detector systems. Using the measured storage lifetimes we estimate that the residual gas pressure is in the 10(-14) mbar range. When high current ion beams are injected, the number of stored particles does not follow a single exponential decay law as would be expected for stored particles lost solely due to electron detachment in collision with the residual-gas. Instead, we observe a faster initial decay rate, which we ascribe to the effect of the space charge of the ion beam on the storage capacity.

  • 15.
    Seitz, Fabian
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Zettergren, Henning
    Stockholm University, Faculty of Science, Department of Physics.
    Rousseau, P.
    Wang, Y.
    Chen, Tao
    Stockholm University, Faculty of Science, Department of Physics.
    Gatchell, Michael
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Stockett, Mark H.
    Stockholm University, Faculty of Science, Department of Physics.
    Rangama, J.
    Chesnel, J. Y.
    Capron, M.
    Poully, J. C.
    Domaracka, A.
    Mery, A.
    Maclot, S.
    Vizcaino, V.
    Schmidt, Henning T.
    Stockholm University, Faculty of Science, Department of Physics.
    Adoui, L.
    Alcami, M.
    Tielens, A. G. G. M.
    Martin, F.
    Huber, B. A.
    Cederquist, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    Ions colliding with clusters of fullerenes-Decay pathways and covalent bond formations2013In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 139, no 3, article id 034309Article in journal (Refereed)
    Abstract [en]

    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.

  • 16.
    Stockett, Mark H.
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Gatchell, Michael
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Berzins, U.
    Chen, Tao
    Stockholm University, Faculty of Science, Department of Physics.
    Farid, K.
    Stockholm University, Faculty of Science, Department of Physics.
    Johansson, A.
    Stockholm University, Faculty of Science, Department of Physics.
    Kulyk, Kostiantyn
    Stockholm University, Faculty of Science, Department of Physics.
    Rousseau, P.
    Stochkel, K.
    Adoui, L.
    Hvelptund, P.
    Huber, B. A.
    Schmidt, Henning T.
    Stockholm University, Faculty of Science, Department of Physics.
    Zettergren, Henning
    Stockholm University, Faculty of Science, Department of Physics.
    Cederquist, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    Fragmentation of anthracene C14H10, acridine C13H9N and phenazine C12H8N2 ions in collisions with atoms2014In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 16, no 40, p. 21980-21987Article in journal (Refereed)
    Abstract [en]

    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.

  • 17.
    Thomas, Richard D.
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Schmidt, Henning T.
    Stockholm University, Faculty of Science, Department of Physics.
    Gatchell, Michael
    Stockholm University, Faculty of Science, Department of Physics.
    Rosén, Sara
    Stockholm University, Faculty of Science, Department of Physics.
    Reinhed, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Löfgren, Patrik
    Stockholm University, Faculty of Science, Department of Physics.
    Brännholm, Lars
    Stockholm University, Faculty of Science, Department of Physics.
    Blom, Mikael
    Stockholm University, Faculty of Science, Department of Physics.
    Björkhage, Mikael
    Stockholm University, Faculty of Science, Department of Physics.
    Bäckström, Erik
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Leontein, Sven
    Stockholm University, Faculty of Science, Department of Physics.
    Hanstorp, D.
    Zettergren, Henning
    Stockholm University, Faculty of Science, Department of Physics.
    Kaminska, Magdalena
    Stockholm University, Faculty of Science, Department of Physics.
    Nascimento, Rodrigo
    Stockholm University, Faculty of Science, Department of Physics.
    Liljeby, Leif
    Stockholm University, Faculty of Science, Department of Physics.
    Källberg, Anders
    Stockholm University, Faculty of Science, Department of Physics.
    Simonsson, Ansgar
    Stockholm University, Faculty of Science, Department of Physics.
    Hellberg, Fredrik
    Stockholm University, Faculty of Science, Department of Physics.
    Mannervik, Sven
    Stockholm University, Faculty of Science, Department of Physics.
    Larsson, Mats
    Stockholm University, Faculty of Science, Department of Physics.
    Geppert, Wolf D.
    Stockholm University, Faculty of Science, Department of Physics.
    Rensfelt, Karl-Gunnar
    Stockholm University, Faculty of Science, Department of Physics.
    Paál, Andras
    Stockholm University, Faculty of Science, Department of Physics.
    Masuda, Masaharu
    Stockholm University, Faculty of Science, Department of Physics.
    Halldén, Per
    Stockholm University, Faculty of Science, Department of Physics.
    Andler, Guillermo
    Stockholm University, Faculty of Science, Department of Physics.
    Stockett, Mark H.
    Stockholm University, Faculty of Science, Department of Physics.
    Chen, Tao
    Stockholm University, Faculty of Science, Department of Physics.
    Källersjö, Gunnar
    Stockholm University, Faculty of Science, Department of Physics.
    Weimer, Jan
    Stockholm University, Faculty of Science, Department of Physics.
    Hansen, K.
    Hartman, H.
    Cederquist, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    DESIREE: Physics with cold stored ion beams2015In: DR2013: Ninth international conference on dissociative recombination: theory, experiment, and applications, 2015, Vol. 84, article id 01004Conference paper (Refereed)
    Abstract [en]

    Here we will briefly describe the commissioning of the Double ElectroStatic Ion Ring ExpEriment (DESIREE) facility at Stockholm University, Sweden. This device uses purely electrostatic focussing and deflection elements and allows ion beams of opposite charge to be confined under extreme high vacuum and cryogenic conditions in separate rings and then merged over a common straight section. This apparatus allows for studies of interactions between cations and anions at very low and well-defined centre-of-mass energies (down to a few meV) and at very low internal temperatures (down to a few K).

  • 18.
    Zettergren, Henning
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Rousseau, P.
    Wang, Y.
    Seitz, Fabian
    Stockholm University, Faculty of Science, Department of Physics.
    Chen, Tao
    Stockholm University, Faculty of Science, Department of Physics.
    Gatchell, Michael
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Stocket, Mark H.
    Stockholm University, Faculty of Science, Department of Physics.
    Rangama, J.
    Chesnel, J. Y.
    Capron, M.
    Poully, J. C.
    Domaracka, A.
    Mery, A.
    Maclot, S.
    Schmidt, Henning T.
    Stockholm University, Faculty of Science, Department of Physics.
    Adoui, L.
    Alcami, M.
    Tielens, A. G. G. M.
    Martin, F.
    Huber, B. A.
    Cederquist, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    Formations of Dumbbell C-118 and C-119 inside Clusters of C-60 Molecules by Collision with alpha Particles2013In: Physical Review Letters, ISSN 0031-9007, E-ISSN 1079-7114, Vol. 110, no 18, article id 185501Article in journal (Refereed)
    Abstract [en]

    We report highly selective covalent bond modifications in collisions between keV alpha particles and van der Waals clusters of C-60 fullerenes. Surprisingly, C-119(+) and C-118(+) are the dominant molecular fusion products. We use molecular dynamics simulations to show that C-59(+) and C-58(+) ions-effectively produced in prompt knockout processes with He2+-react rapidly with C-60 to form dumbbell C-119(+) and C-118(+). Ion impact on molecular clusters in general is expected to lead to efficient secondary reactions of interest for astrophysics. These reactions are different from those induced by photons.

  • 19.
    Zettergren, Henning
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Rousseau, P.
    Wang, Y.
    Seitz, Fabian
    Stockholm University, Faculty of Science, Department of Physics.
    Chen, Tao
    Stockholm University, Faculty of Science, Department of Physics.
    Gatchell, Michael
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Stocket, Mark H.
    Stockholm University, Faculty of Science, Department of Physics.
    Rangama, J.
    Chesnel, J. Y.
    Capron, M.
    Poully, J. C.
    Domaracka, A.
    Méry, A.
    Maclot, S.
    Schmidt, Henning T.
    Stockholm University, Faculty of Science, Department of Physics.
    Adoui, L.
    Alcamí, M.
    Tielens, A. G. G. M.
    Martín, F.
    Huber, B. A.
    Cederquist, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    Formation of dumb-bell C118 and C119 inside clusters of C60 -moleculesArticle in journal (Refereed)
    Abstract [en]

    We report highly selective covalent bond-modifications in collisions between keV alpha particles and van der Waals clusters of C60-fullerenes. Surprisingly, C119+ and C118+ are the dominant molecular fusion products. We use Molecular Dynamics simulations to show that C59+ and C58+ ions - effectively produced in prompt knock-out processes with He2+ - react rapidly with C60 to form dumb-bell C119+ and C118+ . Ion impact on molecular clusters in general is expected to lead to efficient secondary reactions of interest for astrophysics. These reactions are different from those induced by photons.

  • 20.
    Zettergren, Henning
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Rousseau, P.
    Wang, Y.
    Seitz, Fabian
    Stockholm University, Faculty of Science, Department of Physics.
    Chen, Tao
    Stockholm University, Faculty of Science, Department of Physics.
    Gatchell, Michael
    Stockholm University, Faculty of Science, Department of Physics.
    Alexander, John D.
    Stockholm University, Faculty of Science, Department of Physics.
    Stockett, Mark H.
    Stockholm University, Faculty of Science, Department of Physics.
    Rangama, J.
    Chesnel, J. Y.
    Capron, M.
    Poully, J. C.
    Domaracka, A.
    Mery, A.
    Maclot, S.
    Vizcaino, V.
    Schmidt, Henning T.
    Stockholm University, Faculty of Science, Department of Physics.
    Adoui, L.
    Alcami, M.
    Tielens, A. G. G. M.
    Martin, F.
    Huber, B. A.
    Cederquist, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    Bond formation in C-59(+)-C-60 collisions2014In: XXVIII International Conference on Photonic, Electronic and Atomic Collisions (ICPEAC 2013), Institute of Physics (IOP), 2014, article id 012028Conference paper (Refereed)
    Abstract [en]

    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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