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  • 1
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 106 (1997), S. 9067-9077 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Vibrational excitation of an Ar55 cluster in collisions with He (Ekin=25 meV) is investigated by using classical trajectories and a highly approximate quantum mechanical method (vibrationally sudden approximation). The energy transfer from the helium atom to the cluster (ΔE) is calculated as a function of the scattering angle θ. It is found (i) that predominantly the modes corresponding to the cluster atoms in the outer shell are excited and (ii) that the probability for multi-phonon (Δn≥2) excitations steadily increases with the scattering angle. The results of both sets of calculations are generally in good agreement with measured energy loss spectra over the entire range of scattering angles. In the region θ(approximate)15°–30°, which—because single-phonon transitions dominate—is most important for determining the frequency distribution of the cluster, the quantum mechanical calculations are superior to classical mechanics; the latter fails to conserve zero-point energy and therefore leads to unrealistic energy transfer below ΔE(approximately-less-than)2 meV. © 1997 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 106 (1997), S. 6795-6805 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The structures of small hydrazine clusters from the dimer to the hexamer have been calculated using a standard site-site intermolecular potential and a newly developed systematic approach which is essentially based on monomer properties. Aside from the repulsive and the attractive dispersion and induction interaction special care is taken for the determination of the electrostatic interaction which is represented by a distributed multipole expansion and a penetration correction. Based on these potentials the vibrational spectra of the N-N stretching and the asymmetric NH2 wagging mode are calculated using degenerate perturbation theory. While the small shifts of the N-N stretching mode are fairly well reproduced by both potential models, large differences are predicted for the asymmetric NH2 wagging mode. Here, redshifts of –30 cm−1 are calculated for the standard and blueshifts of 100 cm−1 are obtained for the systematic potential in agreement with experiment. The analysis shows that the reason for this behavior is the careful treatment of the electrostatic term in this model. © 1997 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 111 (1999), S. 10069-10076 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Helium atoms are scattered from a beam of water clusters with mean size n¯ = 10 in an angular and velocity resolved collision experiment. The measured peaks are identified as elastic scattering, rotationally inelastic scattering of monomers, and vibrational excitation of the clusters. To interpret the latter processes quantum calculations are performed for He+(H2O)11 collisions using the TDSCF approximation which includes the anharmonic force field of the water clusters and energy transfer between the modes. By comparison of the calculated and experimental results, the most probable excitations correspond to energy transfer for around 7 meV and, with smaller intensities, up to 20 meV. The excitations correspond to shearing modes of the outer rings and the middle ring of the highly nonrigid cluster against each other. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 4
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 106 (1997), S. 3205-3215 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: In a crossed molecular beam arrangement helium atoms are scattered from argon clusters which are generated in the size range of n¯=23 to n¯=4600 by adiabatic expansion with conical nozzles. The inelastic energy transfer is detected by time-of-flight analysis of the scattered helium atoms with a resolution of better than 1 meV. The angular dependence allows to distinguish between single and multiphonon excitations. The measured peaks of the averaged transferred energy in the single phonon regime decrease with increasing average cluster size and converges to the values of the surface phonons of solid argon. This behavior is explained by treating the data as collective breathing vibrations of a solid sphere. © 1997 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 5
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 106 (1997), S. 6806-6812 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Vibrational predissociation spectra of hydrazine (N2H4)n clusters have been measured from the dimer to the tetramer using a linetunable, isotopically substituted CO2-laser in order to fill the frequency gap between 990 and 1010 cm−1. The clusters are size selected in a scattering experiment with helium atoms. The large blue shifts of the asymmetric NH2 wag mode at 937 cm−1 are completely interpreted by calculations based on a recently determined systematic model potential. The gross shifts of 60 cm−1 for the dimer, 80 cm−1 for the trimer, and 110 cm−1 for the larger clusters are explained by the different structures: Cyclic arrangements with two hydrogen bonds per molecule for the dimer, rings with one hydrogen bond per molecule for the trimer, and three-dimensional structures for the larger ones. The peaks in the spectra are caused by characteristic vibrations to which more than one isomer contributes. © 1997 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 6
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Review of Scientific Instruments 63 (1992), S. 3936-3938 
    ISSN: 1089-7623
    Source: AIP Digital Archive
    Topics: Physics , Electrical Engineering, Measurement and Control Technology
    Notes: A supersonic sodium cluster beam source with a refilling system is described in detail. Due to the external refilling system a new loading of the oven, which is designed for high-temperature application at 800 °C, is accomplished very fast and interrupts the measuring process only for 1–2 h. Additional purification of the alkali metal in the reservoir allows the usage of standard quality sodium samples.
    Type of Medium: Electronic Resource
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  • 7
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Review of Scientific Instruments 67 (1996), S. 417-422 
    ISSN: 1089-7623
    Source: AIP Digital Archive
    Topics: Physics , Electrical Engineering, Measurement and Control Technology
    Notes: We describe the advantages of using the pseudorandom time-of-flight (TOF) technique for measuring velocity distributions together with the TOF mass spectrometric detection. The basic idea of the method is the successive measurement of abundance spectra with the TOF mass spectrometer correlated with each channel of the pseudorandom sequence. Extraction of the intensities of each mass and subsequent cross correlation with the pseudorandom sequence leads to the TOF and thus the velocity distributions. The proposed technique can substantially reduce the data acquisition time in systems for which many different reaction products are expected such as in cluster research. An illustration of the efficiency is presented using angular resolved TOF distributions for products of the reaction of sodium clusters Nan with O2. © 1996 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 8
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 82 (1985), S. 202-216 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: In a crossed molecular beam experiment differential energy loss spectra have been measured for Xe+CO2 collisions at energies of 0.2, 0.58, 1.0, and 1.6 eV. Nearly the complete angular range from 40° to 180° in the center-of-mass system was covered. At large deflection angles and small energy transfers (Δ E/E(approximately-equal-to)0.1) the spectra exhibit a large intensity peak which cannot be explained by usual rotational rainbow theory. Quantum and classical calculations in the centrifugal sudden approximation demonstrate that this effect is a multiple collision rotational rainbow. In the first collision the kinetic energy is nearly completely transferred to rotational energy of the CO2 molecule. Since the heavy Xe atom leaves the interaction region very slowly, a second collision occurs and the rotational motion is deaccelerated. The classical excitation function J (γi), which relates the final angular momentum with the orientation angle of the molecule, has three extrema, two of which give rise to the multiple collision rotational rainbow. Various test calculations show that the effect depends strongly on the reduced mass, on the anisotropy and, in contrast to the normal rotational rainbow, also on the slope of the repulsive part of the interaction potential. Exact three-dimensional classical trajectory calculations at E=1.0 eV based on a realistic model potential agreed satisfactorily with the experimental results.
    Type of Medium: Electronic Resource
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  • 9
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 87 (1987), S. 6276-6283 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Ethylene clusters (C2H4)n are generated in a supersonic expansion with He and size selected by scattering from a helium beam. The clusters are dissociated upon absorption of a photon from a pulsed CO2 laser by exciting the ν7 mode of the monomer. During the collision about 30 meV of internal energy is transferred to the cluster so that the laser photons interact with internally hot clusters. The frequency and fluence dependences of the photodissociation cross sections are measured for (C2H4)n with n=2,3,4,5, and 6. Nearly all spectra exhibit structure which is most pronounced for the dimer. The overall width (FWHM) decreases from 31.2 cm−1 for the dimer to 12.2 cm−1 for the hexamer, while the maximum position is nearly the same (951.6 cm−1). The structure of the dimer spectrum is attributed to hot bands. The large linewidth corresponds to a short lifetime in the ps range.
    Type of Medium: Electronic Resource
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  • 10
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 84 (1986), S. 4854-4861 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Arn clusters generated in a supersonic nozzle beam are investigated by exploiting their different kinematical behavior in a scattering experiment. In a crossed molecular beam experiment the Arn clusters are scattered from He atoms at E=69.7 meV. By measuring the angular and velocity distributions of the scattered clusters, the different species can be separated from each other. In this way fragmentation probabilities of small Arn clusters up to n=6 by electron impact ionization are measured. The influence of collisional dissociation of the dimer is accounted for by classical trajectory calculations. The dimer fragmentation is found to be f21=0.40±0.05, while the trimer totally fragments to dimers ( f32=0.7±0.3) and monomers ( f31=0.3). All clusters with n from 4 to 6 appear with a probability of 0.95 on the dimer ion mass.
    Type of Medium: Electronic Resource
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