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  • 1
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 102 (1995), S. 7610-7621 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The method of thermodynamic integration is used to determine the free energy of the restricted primitive model of electrolytes along two subcritical isotherms. The densities of liquid-gas coexistence derived from these data are found to be in good agreement with recent estimates from Gibbs ensemble Monte Carlo calculations. The difficulties of the free energy approach—which reside in the necessity of obtaining extremely accurate free energy values at near critical temperatures—is stressed. A detailed account is given of the clustering properties of the ions in the vapor phase, including cluster populations and energies, as well as intercluster contributions to the thermodynamic properties. The validity of several cluster theories for the free energy is investigated. © 1995 American Institute of Physics.
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  • 2
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 105 (1996), S. 1101-1112 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We report Monte Carlo (MC) simulations for the pair correlation functions of a hard sphere fluid in a hard sphere matrix. In particular, we evaluate the blocking function hb(r) which is that part of the fluid pair correlation function which accounts for the correlation between fluid particles mediated through at least one matrix particle. The results are compared with integral equation theory. A scheme for determining the bridge functions is presented which predicts excellent agreement of the pair structure with MC results. © 1996 American Institute of Physics.
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  • 3
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 103 (1995), S. 3820-3831 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: This paper reports a Monte Carlo (MC) study of the ordering in a semiflexible liquid crystal model designed to give a crude representation of 4-n-octyl-4′-cyanobiphenyl (PCB). A mechanically stable nematic phase is obtained and the question of its thermodynamic stability is addressed by comparing the free energy to that of the isotropic phase. The free energies are calculated by thermodynamic integration using an efficient configuration biased MC scheme. Pair distribution functions, orientational correlation functions, and conformational properties of the nematic and isotropic phases are contrasted. In the isotropic phase the equation of state is compared with theoretical predictions for systems of convex molecules and chains made up of tangent hard spheres. © 1995 American Institute of Physics.
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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. 6107-6115 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The mechanical stability of two different smectic arrangements formed by molecules having a rigid core and a semiflexible tail has been investigated by Monte Carlo simulation as a function of temperature, pressure, and chain length. © 1997 American Institute of Physics.
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  • 5
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 109 (1998), S. 7486-7497 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A model system of electrolytes, the three-dimensional restricted primitive model (RPM), is investigated for the case where the charged hard spheres are constraint to move on a two-dimensional surface. The properties of the thermodynamic states corresponding to the gas and liquid phases have been determined by computer simulation for a wide range of densities and temperatures. The simulations provide results for the equation of state, internal energy, and correlation functions of the 3D RPM confined to 2D, and allow a characterization of the local order of the charged spheres as a function of density and temperature. The most striking aspect of this order is the organization, at low, although supercritical, temperature and low to moderate densities, of the spheres into "clusters" where linear arrangements or chains of alternatively positive and negative charges dominate. The domain of validity of the hypernetted chain integral equation is investigated. The critical temperature of the gas–liquid transition is located with precision by means of a finite size scaling analysis of the simulation results in the critical region. With regard to the critical behavior of the 2D RPM, the limitations on system sizes which could be studied do not allow to conclude more than possible compatibility with the 2D Ising universality class. © 1998 American Institute of Physics.
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  • 6
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 104 (1996), S. 3629-3637 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The interaction of C+60 and C+70 ion beams with a surface of highly oriented pyrolitic graphite was investigated by probing the ionization and fragmentation rates of scattered species within a time window of 20 μs following impact. Neutralization/reionization and fragmentation behavior was observed and followed by a pulsed deflection field applied to the surface at variable delays after the collision event. An almost complete collisional neutralization of the incident projectile was found. For an impact energy of 140–180 eV, a significant part of the scattered species was found to reionize by delayed electron emission within the experimental time window. The associated reionization and fragmentation kinetics were modeled with a system of differential equations assuming a simple unimolecular reaction diagram. Rate constants for delayed ionization and fragmentation were calculated as functions of internal energy and respective activation energies with the "finite heat bath'' model (Klots) and the Rice–Ramsperger–Kassel–Marcus expression, respectively. The calculated and measured (deflection field delay dependent) ion intensities were compared in a fit procedure. The best fit led to an activation energy for the fragmentation of C+60 (C+60→C+58+C2) of 6.6±0.5 eV. This translates to an activation energy of 7.1±0.5 eV for the fragmentation of neutral C60 (using the experimentally determined ionization potential of C58). For C+70 we obtained an identical (within error) activation energy for fragmentation (C+70→C+68+C2) of 6.6±0.5 eV. © 1996 American Institute of Physics.
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  • 7
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 104 (1996), S. 3638-3650 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Fragmentation of various fullerenes was studied by surface impact on highly oriented pyrolytic graphite at collision energies Ecol of 150–1050 eV/molecule. The projectiles C+60, C+70, C+76, C+84, and C+94 were formed by laser desorption of chromatographically separated samples, while large carbon clusters C+94, C+110, C+164 were produced by laser-induced coalescence reactions. Except at the highest impact energies, the fragment distributions consist of even numbered C+n species with abundance maxima similar to those observed in fullerene synthesis. With increasing Ecol, we observe a size evolution in the fragment distributions characteristic of a sequential fragmentation process. Simulated fragment distributions based on statistical rate theory and a sequential C2 loss mechanism reproduce the experimental data well up to a maximum Ecol. They are used to determine the mean energy transfer during surface impact as a function of collision energy as well as its dependence on several experimental parameters such as the nature (cleanliness) of the target surface, the internal energy of the incident ion, and the incident fullerene size. Both internal and kinetic energy of the incident ion are found to contribute to the observed fragmentation although with different efficiencies. For the higher fullerenes we find a tendency towards increasing transfer efficiency of incident kinetic to internal energy with increasing projectile size. Finally, above a size-dependent impact energy threshold, a transition to a different high energy fragmentation process is indicated by changes in the fragment distributions. These go from exclusively even numbered fullerene fragments at low impact energy to smaller even and odd numbered C+n fragments at high Ecol. It is suggested that this change indicates the formation of high energy, nonfullerene isomers. © 1996 American Institute of Physics.
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  • 8
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Review of Scientific Instruments 67 (1996), S. 3248-3251 
    ISSN: 1089-7623
    Source: AIP Digital Archive
    Topics: Physics , Electrical Engineering, Measurement and Control Technology
    Notes: Construction details of a low-temperature raster system for moving crystals with a maximum size of 14 mm × 14 mm × 14 mm over a small area of piezoelectric sound excitation are described. The pure mechanical raster system in the liquid helium is driven by two stepping motors outside the cryostat. The minimum step size is 1 μm and the maximum raster area 14 mm×14 mm. This raster system was used in sound-beam topography at a frequency of 70 GHz. For this purpose, a special quasioptical transmission line across the dewar wall was also developed which is briefly described together with the applied electromechanical transducer system. © 1996 American Institute of Physics.
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  • 9
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Review of Scientific Instruments 66 (1995), S. 4188-4197 
    ISSN: 1089-7623
    Source: AIP Digital Archive
    Topics: Physics , Electrical Engineering, Measurement and Control Technology
    Notes: A new tandem time-of-flight mass spectrometer is described which is designed to study the mass-, velocity-, and angle-resolved scattering of cluster ions from solid surfaces. Clusters are produced in a supersonic jet laser desorption/vaporization source, ionized either directly in the formation step or by subsequent photoionization of neutrals, mass selected in a primary time-of-flight region, and decelerated to the impact energy (50–1000 eV) close to the target surface. Cluster–surface collisions take place in a field-free region in order to determine both velocity and angular distributions of the scattered clusters and fragments with an independently pulsed, rotatable secondary time-of-flight mass spectrometer. Several surface targets can be mounted in the UHV scattering chamber (10−10 Torr base pressure) on a five-axis manipulator which, together with the rotatable secondary TOF, allows for independent variation of incident and scattering angles. Target surfaces can be cleaned by direct current heating and sputtering with an argon-ion gun. Surface structure and composition are assessed by low-energy electron diffraction (LEED) and Auger spectroscopy with a four grid reverse view LEED/Auger system. Surface collision experiments of fullerenes (C+60, C+70, C+76, C+84, ...) and metallofullerenes (La@xaC+82) with highly oriented pyrolitic graphite (HOPG) surfaces are described as examples for the performance of the instrument. Effects of surface contamination in the scattering of fullerenes from HOPG are described to demonstrate the need for thorough cleaning procedures in order to obtain reproducible results. © 1995 American Institute of Physics.
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  • 10
    ISSN: 1089-7623
    Source: AIP Digital Archive
    Topics: Physics , Electrical Engineering, Measurement and Control Technology
    Notes: Conventional zero-field optically detected magnetic resonance (ODMR) is normally performed by using a slow-wave helix for microwave excitation with a quality factor Q(approximate)1. With available microwave sources this low Q factor leads to long microwave pulse lengths for coherent pulse experiments (π-pulse duration of about 300 ns for 20 W microwave excitation power). For our zero-field experiments we took advantage of the bridged loop-gap microwave resonator configuration with relatively high Q factor. Without the possibility of tuning the Zeeman energy level splitting as in electron paramagnetic resonance (EPR), in zero-field ODMR the resonator has to cover a wide range of frequencies. We are able to tune our probehead in the range of 1.9–8 GHz with a loaded Q factor of up to 800 by using interchangeable bridged loop-gap resonators of various designs. Thereby, the pulse lengths, compared to the slow-wave helix, could be reduced by nearly one order of magnitude (tresonatorπ=45 ns employing the same microwave power of 20 W). Experimental data are presented for triplet states of photoexcited acridine and benzophenone molecules at different resonance frequencies for their |Tx〉−|Tz〉 transitions (ν=2.472 GHz and ν=5.226 GHz), respectively. © 1997 American Institute of Physics.
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