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  • 1
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 105 (1996), S. 1880-1896 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Electron impact ionization of C60 and C70 was studied using a molecular/electron beam ion source in combination with a two sector field mass spectrometer operated in the ion beam deflection mode. Relative partial ionization cross sections for the production of singly and multiply charged parent ions (up to charge state z=4) and fragment ions (down to C+44 in the case of C60 and down to C2+50 in the case of C70) were determined from threshold up to 1000 eV electron energy. Absolute partial and total ionization cross sections are obtained using a novel approach for the absolute calibration involving an intercomparison of the cation with the anion yield. The results obtained reveal not only an anomalous large parent ion cross section as compared to other ionization channels [e.g., σ(C+60/C60) is more than a factor of 30 larger than σ(C+58/C60)] but also anomalies for the production of multiply charged parent and fragment ions. For instance, the maximum cross section for the formation of C2+60 amounts to 30% of the maximum C+60 cross section and that of C2+70 to about 50% of C+70. Moreover, for all fragment ions, the formation of the doubly charged fragment ions has a larger cross section than that of the respective singly charged fragment ion. These peculiar features of the kinetics of electron impact ionization of C60 and C70 are related to the specific electronic and geometric structures of these fullerenes. The present absolute cross-section data for the summed up partial cross sections are in good agreement with a recent semiclassical calculation from our laboratory. © 1996 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 2
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 111 (1999), S. 3548-3558 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Highly monochromatized electrons (with energy distributions of less than 30 meV FWHM) are used in a crossed beam experiments to investigate electron attachment to oxygen clusters (O2)n at electron energies from approximately zero eV up to several eV. At energies close to zero the attachment cross section for the reaction (O2)n+e→(O2)m− (for m=1, 2, and 3) rises strongly with decreasing electron energy compatible with s-wave electron capture to (O2)n. Peaks in the oxygen attachment cross sections present at higher energies ((approximate)80 meV, 193 meV, 302 meV) can be ascribed to vibrational levels of the anion populated by attachment of an electron to a single oxygen molecule within the target cluster via a direct Franck–Condon transition from the ground vibrational state v=0 to a vibrational excited state v′=7,8,9,... of the anion produced. The vibrational structures observed here for the first time can be quantitatively accounted for by model calculations using a microscopic model to examine the attachment of an electron to an oxygen molecule inside a cluster. This involves (i) molecular dynamics simulations to calculate the structure of neutral clusters prior to the attachment process and (ii) calculation of the solvation energy of an oxygen anion in the cluster from the electrostatic polarization of the molecules of the cluster. The occurrence of this polarization energy at the surface of larger clusters explains the appearance of an s-wave capturing cross section at 0 eV and the slightly smaller spacings (compared to the monomer case) between the peaks at finite energy, as observed experimentally. The relative transition probabilities from the ground state of the neutral oxygen molecule to the different vibrational levels of the anion are obtained by calculating the corresponding Franck–Condon factors thereby resulting in a reasonable theoretical fit to the observed yields of negatively charged oxygen molecules and clusters. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 3
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 107 (1997), S. 8955-8962 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Using a crossed electron-molecule beam ion source in combination with a quadrupole mass spectrometer we have studied the electron energy dependence of the dissociative attachment process CHCl3+e→Cl− at electron energies from about 0 to 2 eV and in a target gas temperature range of about 300–430 K. The energy resolution and working conditions of this newly constructed crossed beams machine have been characterized using CCl4 as a test and calbrant gas. Utilizing the improved energy resolution of the present experimental setup (which allows measurements with FWHM energy spreads down to below 5 meV) it was possible to determine the accurate shape and magnitude of the cross section function in the low-energy range. This leads to the conclusion that between an electron energy of about 20 and 130 meV the reaction proceeds via deBroglie s-wave capture, whereas at higher energy (above about 0.4 eV) autodetachment plays a significant role. Moreover, the present measurements allow us to clarify previously reported differences in the absolute cross section, the number of peaks and in the energy position of these peaks. Finally, by analyzing the measured strong temperature dependence of the cross section close to zero electron energy the activation barrier for this dissociative attachment was determined to be 110±20 meV in good agreement with thermochemical data from swarm experiments performed under thermal equilibrium. Taking into account the present results it is also possible to discuss the mechanism for the existence of the second peak. © 1997 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 4
    Electronic Resource
    Electronic Resource
    Springer
    Czechoslovak journal of physics 48 (1998), S. 1135-1145 
    ISSN: 1572-9486
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract The 4.4eV dissociative electron attachment peak in CO2 was reinvestigated paying particular attention to (i) its structure associated with vibrational excitation and to (ii) the temperature dependence of the onset. For this purpose we have used two specially designed crossed beams machines, one having a trochoidal electron analyzer (TEM) and one with a hemispherical electron analyzer (HEM) for the production of the highly monochromatized electron beams (with FWHM's down to 5 and 50meV, respectively). The present results confirm the earlier findings in (i) interpreting the dominant structures of the 4.4eV peak as being due to vibrationally excited states of CO in the reaction CO2 + e → O-+ CO and (ii) assigning the much weaker and narrower structures to the intermediate CO 2 - . In the temperature range between 300 and 245 K almost no temperature dependence of the onset can be seen in the present study. In comparison to NO and CO where the onset is vertical the CO2 threshold behavior is less steep indicating that in the CO2 case a different type of transition must be responsible for the onset of the O− production. Besides DA to CO2 we have for comparison and calibration purposes investigated also DA to CO and NO.
    Type of Medium: Electronic Resource
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  • 5
    Electronic Resource
    Electronic Resource
    Springer
    Czechoslovak journal of physics 49 (1999), S. 383-392 
    ISSN: 1572-9486
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract Using a recently constructed high resolution crossed electron/molecular beam apparatus consisting of a hemispherical electron monochromator and a quadrupole mass spectrometer we have measured the relative production cross sections for CI– and F– via electron attachment to CF2Cl2. The relative Cl– cross section is placed on an absolute scale by reference to an absolute rate coefficient using a calibration method involving integration of the measured anion signal. The most efficient Cl– production process is at about zero energy and its magnitude is resolution limited. The present high resolution value of 6 × 10−16 cm2 compares well with an earlier value reported by Chen and Chantry. A second peak is detected at around 0.8 eV in accordance with some of the earlier beam and swarm measurements. The observed production of F– has an appearance energy of 1.9 eV and the energy of maximum cross section is 3.36 eV, the latter value comparing well with several previous studies.
    Type of Medium: Electronic Resource
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  • 6
    ISSN: 1434-6079
    Keywords: PACS: 36.40.-c Atomic and molecular clusters – 34.80.Lx Electron–ion recombination and electron attachment
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract. The formation of both positively and negatively charged ions after interaction of electrons with different cluster beams is investigated, by the use of highly monochomatized electron beams. In the case of the electron attachment to neutral NO clusters, the formation of the monomer ion NO- could be observed for the first time. The only explanation for the creation of such an ion is an intracluster reaction. In the case of carbon monoxide clusters, the appearance energies were determined with high accuracy. From these data, we derived the binding energy of the cluster dimer. Our results are in good agreement with photoionization studies.
    Type of Medium: Electronic Resource
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  • 7
    ISSN: 1434-6079
    Keywords: 36.40
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract Stoichiometric and non-stoichiometric, positive and negative oxygen cluster ions (n up to 70) have been produced in a crossed neutral beam/electron beam ion source. The abundance and stability of the ions formed have been analyzed with a double focussing sector field mass spectrometer in a series of experiments. Positive and negative ion mass spectra observed exhibit distinct abundance anomalies, however, at different cluster sizes. Abundance maxima and minima correlate with correspondingly small and large metastable fractions of (O2) n + and (O2) n − ions, respectively. (O2) n + ions may also lose up top=(n−1) monomers by collision induced dissociation with monotonously decreasing probability with increasingp. Metastable fractions determined for (O2) n − ions produced with appr. zero eV electrons are in general larger than those for ions produced with appr. 7 eV electrons. (O2) n − ions are also observed to decay via autodetachment, with lifetimes increasing with increasing cluster size. Finally, here we were able to prove that an apparent loss of the monomer fragment O (and higher homologues) observed in the metastable time regime is due to ordinary metastable monomer evaporation in the acceleration region. Moreover, we will also present here some new data and interpretation concerning the electron attachment cross section function for O2 clusters.
    Type of Medium: Electronic Resource
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  • 8
    Electronic Resource
    Electronic Resource
    New York, NY : Wiley-Blackwell
    Rapid Communications in Mass Spectrometry 5 (1991), S. 51-57 
    ISSN: 0951-4198
    Keywords: Chemistry ; Analytical Chemistry and Spectroscopy
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Physics
    Notes: A review of mass spectrometric methods used to study different kinds of clusters is presented. These methods have proved to be indispensable in the cluster field owing to their great flexibility, sensitivity and wide dynamic range. This reviews presents new mass spectrometric methods and techniques such as quadrupole analysers and RF lenses, different ion-trap geometries, time-of-flight (TOF) methods including the reflectron geometry). A variety of ionization methods, both for the production of positive and negative ions, with different amounts of released excess energy, are discussed in detail. Special attention is given to different degree of post-ionization fragmentaqtion and metastability of ions produced by the respective ionization methods. The ability to follow the metastable decay processes in rather different time-windows is also one of the salient features of the mass spectrometric methods reviewed here, involving both classical and new geometries. Detection of very large cluster ions by conventional methods is not always effective, and alternative methods like post-acceleration and using a conversion dynode in front of the multiplier will be included here. Moreover, mass spectrometric methods offer the possibility of producing beams of mass-selected cluster ions necessary for the study of a whole line of process like optical spectrometry, photodetachment, photofragmentation, photoionization, electron beam ionization, and charge-exchange processes. Examples of these processes are also discussed in this review.
    Additional Material: 6 Ill.
    Type of Medium: Electronic Resource
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