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  • 1
    Digitale Medien
    Digitale Medien
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 91 (1989), S. 3240-3245 
    ISSN: 1089-7690
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: Kr clusters produced in a supersonic nozzle expansion have been studied by electron impact ionization mass spectrometry. Mass resolved spectra (with n up to 180) show two homologous series consisting of Kr+n and Kr2+n ions. The distribution of Kr+n ions shows distinct magic number effects, the observed abundance anomalies being very similar to the ones observed in Ar and Xe. This confirms the superior stability of closed-shell and -subshell icosahedral structures. Moreover, we have found evidence for the occurrence of Kr3+n and Kr4+n ions. It was possible to determine appearance sizes of these multiply charged cluster ions (yielding n2=69, n3=156, and n4=264), and to study the electron energy dependence of singly and doubly charged cluster ions (yielding a linear threshold law). These results are discussed in view of various theoretical considerations and previous results where available.
    Materialart: Digitale Medien
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  • 2
    Digitale Medien
    Digitale Medien
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 89 (1988), S. 295-301 
    ISSN: 1089-7690
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: Metastable decay of Ar+@B|3 produced by electron impact ionization of a supersonic Ar cluster beam has been investigated qualitatively and quantitatively with a double focusing sector field mass spectrometer. We present direct experimental proof that the observed metastable decay of Ar+*3 into Ar+ in the microsecond time regime proceeds predominantly via a sequential decay series Ar+@B|3→k3,2Ar+*2→ k2,1Ar+ involving the evaporation of a single monomer in each of these successive decays. The metastable decay rates deduced are very different, i.e., k3,2 =45 s−1 and k2,1 =680 s−1 at an ion acceleration voltage of 3 kV. Moreover, the metastable decay rates of Ar+@B|3 exhibit a strong dependence on time elapsed since electron impact production of the Ar+3, and on ion production parameters (i.e., size and internal excitation energy of the neutral precursor). For instance photodissociation (with visible laser light) of the neutral cluster beam leads to a dramatic increase of the observed metastable reaction rules yielding values of up to 100 000 3−1 in the μs time regime.
    Materialart: Digitale Medien
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  • 3
    Digitale Medien
    Digitale Medien
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 88 (1988), S. 4289-4293 
    ISSN: 1089-7690
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: Clusters of N2 molecules formed in a supersonic nozzle expansion have been studied by electron impact ionization mass spectrometry. Mass resolved spectra (with n up to 190) show three homologous series, i.e., consisting of (N2)+n, (N2)nN+, and [(N2)n N]2+ ions. The distribution of (N2)+n ions shows distinct magic number effects. Moreover, there is evidence for the existence of (N2)2+n and (N2)3+n ions. The critical appearance sizes of observed multiply charged cluster ions are (N2)2+99, (N2)99N2+, and (N2)3+215. These results are compared with theoretical predictions. Moreover, a study of the electron energy dependence of singly and doubly charged N2 cluster ions close to threshold (appearance energies) gives new insight into the ionization mechanism.
    Materialart: Digitale Medien
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  • 4
    Digitale Medien
    Digitale Medien
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 87 (1987), S. 1456-1458 
    ISSN: 1089-7690
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: Clusters of Ne atoms formed in a supersonic nozzle expansion have been studied by electron ionization mass spectrometry. In particular, we have found that the metastable decay of Ne cluster ions is very nonexponential, thus confirming a recent theoretical prediction of Klots applying quasiequilibrium theory to the problem of unimolecular fragmentation of clusters.
    Materialart: Digitale Medien
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  • 5
    Digitale Medien
    Digitale Medien
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 90 (1989), S. 1288-1289 
    ISSN: 1089-7690
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: We report the first well resolved SO2 cluster ion spectrum showing doubly charged parent and fragment ions. The critical appearance size deduced for doubly charged SO2 clusters is n2=21 and for triply charged SO2 clusters n3=49. This result is compared with theoretical predictions.
    Materialart: Digitale Medien
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  • 6
    Digitale Medien
    Digitale Medien
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 88 (1988), S. 6884-6888 
    ISSN: 1089-7690
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: Electron attachment and electron impact ionization of SF6 and SF6/Ar clusters have been investigated in a molecular beam/electron impact ion source/mass spectrometer system. Positive ion mass spectra of neat SF6 clusters contain [(SF6)n⋅SFx]+ fragment ion series with 0≤x≤5 and in addition [(SF6)nS2F5]+ ions which have to be formed via international ion molecule reactions. Positive ion mass spectra of mixed SF6/Ar clusters include ion series of nonstoichiometric fragment ions (SF5⋅Arn)+, (SF6⋅SF5⋅Arn)+, [(SF6)2⋅SF5⋅Arn]+, and, in addition, stoichiometric ions comprised of (SF6⋅Arn)+ and [(SF6)2Arn]+. These stoichiometric ions are only present with n≥3. Electron attachment to neat SF6 clusters gives rise only to stoichiometric (SF6)−n ions, whereas attachment to mixed SF6/Ar clusters yields ion series consisting of (ArnSF6)−, [Arn(SF6)2]−, and [Arn⋅(SF6)3]−. This indicates that the dissociative channel into SF−5 present in the monomer is efficiently quenched in case of clusters. The negative ion mass spectra show in contrast to the positive ion mass spectra a strong dependence on electron energy due to a strong resonance of the attachment cross sections near zero electron energy.
    Materialart: Digitale Medien
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  • 7
    Digitale Medien
    Digitale Medien
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 94 (1991), S. 810-811 
    ISSN: 1089-7690
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: Singly charged argon cluster ions produed by electron impact ionization of a neutral argon cluster beam are found to decay in the metastable time regime by a new mechanism leading to the ejection of "magic'' numbers of neutral argon atoms. The measured dependence of this new decay process on (i) the electron energy, (ii) cluster size and cluster properties, and (iii) the time since ion formation gives insight into the unique mechanism and the nature of this process. At a well-defined threshold energy of ca. 27 eV, the magic number loss mechanism occurs simultaneously with the well-known single monomer evaporation process which proceeds at all energies. Importantly, the new mechanism is the first known example of cluster ion metastability showing an exponential dependence on time, providing further evidence that the precursor parent cluster ion is produced in a specific energy state.
    Materialart: Digitale Medien
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  • 8
    Digitale Medien
    Digitale Medien
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 87 (1987), S. 5238-5241 
    ISSN: 1089-7690
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: Clusters of Ne atoms produced by adiabatic nozzle expansion have been studied with a high resolution double focusing sector field mass spectrometer. Analysis of the isotopic composition of these clusters (up to n=22) showed instead of the expected statistical distribution a pronounced shift to the heavier neon isotope 22Ne. The shift was found to correspond to an increase of the isotope ratio of 22Ne from 8.7% in the monomer to ∼12.5% in the clusters with n〉4 (enrichment factor of ∼1.5.)
    Materialart: Digitale Medien
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  • 9
    Digitale Medien
    Digitale Medien
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 86 (1987), S. 3056-3057 
    ISSN: 1089-7690
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: The electron impact ionization of neutral Ar clusters results in the formation of stable doubly charged Ar2+n only if their size exceeds a critical value. The observed minimum cluster size for argon is Ar2+91 . This result is compared with theoretical predictions.
    Materialart: Digitale Medien
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  • 10
    Digitale Medien
    Digitale Medien
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 116 (2002), S. 984-992 
    ISSN: 1089-7690
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: Electron impact ionization cross sections measured close to threshold are reported for both the monomers and dimers of ozone and OClO using a new high resolution electron impact apparatus. The present appearance energies AE(O3+/O3)=12.70±0.02 eV, AE (OClO+/OClO)=10.55±0.02 and AE(ClO+/OClO=13.37±0.03 eV derived from the measured ionization cross sections are in excellent agreement with the vertical threshold values determined for these ions by high resolution PES and PIMS photoionization studies. The corresponding appearance energies determined for the dimer ions, 10.10±0.3 eV for (O3)2+ and 9.87±0.2 eV for (OClO)2+, are both red shifted with respect to the monomer case. The bond energy (0.70–0.3+0.5) eV of (OClO)2+ estimated from these data is similar to that of other dimer ions, whereas the bond energy of (O3–O3+) with (2.55−0.4+0.6) eV is rather large suggesting an unusual structure for the cationic ozone dimer ion. Based on quantum chemical calculations on various levels we are led to the conclusion that the ion produced by ionization of the ozone dimer is no longer a conventional dimer ion where the two monomer units are still present (as is the case for the OClO system), but rather an ion of form O2(centered ellipsis)O4+ or a twisted ring structure of (O6)+. © 2002 American Institute of Physics.
    Materialart: Digitale Medien
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