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  • 1
    Electronic Resource
    Electronic Resource
    The CO oxidation kinetics on supported Pd model catalysts: A molecular beam/in situ time-resolved infrared reflection absorption spectroscopy study (2001)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 114 (2001), S. 4669-4684 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Combining molecular beam techniques and time-resolved infrared reflection absorption spectroscopy (TR-IRAS) we have studied the kinetics of the CO oxidation reaction on an alumina-supported Pd model catalyst. The Pd particles are deposited by metal evaporation under ultrahigh vacuum (UHV) conditions onto a well-ordered alumina film, prepared on a NiAl(110) single crystal. Particle size, density and structure of the Pd deposits have been characterized in previous studies. In the low temperature region, transient and steady-state experiments have been performed over a wide range of CO and oxygen fluxes by crossing two effusive molecular beams on the sample surface. We determine the steady-state CO2 production rate as a function of the CO fraction in the impinging gas flux. Simultaneously, the occupation of CO adsorption sites under steady-state conditions is monitored by in situ IR spectroscopy. The origin of different types of CO2 transients is discussed. In particular we focus on the transient CO2 production after switching off the CO beam. For the model catalyst investigated, detailed reaction rate measurements in combination with time-resolved IRAS show that the origin of the particular transient behavior of the supported model system is not due to the presence of specific adsorption sites on small particles, as has been proposed previously. Instead, we show that the transient behavior can be semiquantitatively simulated on the basis of a simple kinetic model considering a homogeneous surface, and accounting for the inhibition of the dissociative adsorption of O2 at high CO coverage. Moreover, it is discussed how the inherent heterogeneity of the supported particle system can additionally enhance the observed effect. © 2001 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.1342240
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  • 2
    Electronic Resource
    Electronic Resource
    Collision-induced absorption in the ν2 fundamental band of CH4. II. Dependence on the perturber gas (2002)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 116 (2002), S. 123-127 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The integrated intensities of the collision-induced enhancement spectra of the ν2 band of CH4 perturbed by rare gases and linear molecules (N2, H2, and CO2) are calculated theoretically using the quadrupole transition moment obtained from an analysis of CH4–Ar spectra. In addition to the isotropic quadrupole mechanism responsible for the enhancement in CH4-rare gases, there is additional absorption arising from the anisotropic quadrupole mechanism in the case of molecular perturbers. This latter effect involves the matrix element of the anisotropic polarizability for the ν2 transition in CH4 that is available from the analysis of the depolarized Raman intensity measurements. Overall, the theoretical values for the slope of the enhancement spectra with respect to the perturber density are in reasonably good agreement with the experimental results, thus confirming that the collision-induced absorption arises primarily through the quadrupolar induction mechanism. © 2002 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.1424311
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  • 3
    Electronic Resource
    Electronic Resource
    Line shape parameters for HF in a bath of argon as a test of classical path models (2000)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 113 (2000), S. 9000-9010 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The classical path method proposed by Neilsen and Gordon [J. Chem. Phys. 58, 4131 (1973)] is tested by comparison with extensive fully quantal calculations and recent measurements of cross-sections for HF-Ar. Widths and shifts are found to be in satisfactory agreement both with the close-coupling and experimental results. Comparisons are also made with more "downgraded" theoretical approaches based on the peaking approximation and the neglect of the time ordering. Finally, the Neilsen and Gordon approach is used in order to demonstrate that vibration-rotation coupling significantly contributes to the rotational dependence of both widths and shifts cross-sections. © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.1319346
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  • 4
    Electronic Resource
    Electronic Resource
    Experimental and theoretical study of line mixing in methane spectra. III. The Q branch of the Raman ν1 band (2000)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 112 (2000), S. 1335-1343 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The shape of the ν1 Raman Q branch of CH4 perturbed by Ar and He at room temperature has been studied. Stimulated Raman spectroscopy (SRS) experiments have been made in the 2915–2918 cm−1 spectral region for total pressures from 0.4 to 70 atm and mixtures of (approximate)5% CH4 with He and Ar. Analysis of the spectra demonstrates that the shape of the Q branch is significantly influenced by line mixing and much narrower than what is predicted by the addition of individual line profiles. For the first time, a model is proposed for the calculation and analysis of the effects of collisions on the considered spectra. In this approach, the rotational part of the relaxation matrix is constructed, with no adjustable parameter, starting from semiclassical state-to-state rates. Two empirical constants which account for the shift and broadening of the branch due to vibrational effects are introduced and their values are determined from fits of measured spectra. Comparisons between measurements and results computed with and without the inclusion of line mixing are made. Although not perfect, our model satisfactory accounts for most effects of pressure at low densities, where rotational transfers are dominant, as well as at high densities, where the profile is strongly influenced by vibrational contributions. It is shown that collisions with He and Ar lead to different behaviors at elevated pressure. The influence of the perturbation introduced by the Fermi coupling between the ν1 and ν2+ν4 levels is discussed and the rotational and vibrational contributions to the spectral shape are pointed out. © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.480597
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  • 5
    Electronic Resource
    Electronic Resource
    Experimental and theoretical study of line mixing in methane spectra. IV. Influence of the temperature and of the band (2000)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 113 (2000), S. 5776-5783 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Line-mixing effects are studied in infrared bands of CH4 perturbed by N2 at various pressures. The effects of temperature are investigated in the ν3 region whereas spectral shapes of the ν2, ν4, and ν3 bands are compared at room temperature. The theoretical approach proposed in preceding papers is used in order to model and analyze the influence of collisions on the spectral shape. All model parameters are now fixed to values determined in the previous studies. Comparisons between measurements and spectra computed with and without the inclusion of line mixing are made. They show that our approach satisfactorily accounts for the effects of temperature, pressure, and of rotational quantum numbers on the absorption by the ν3 band. Furthermore, the effects of collisions on spectra in the ν4 region at room temperature are also correctly calculated. On the other hand, the proposed approach fails in modeling the evolution with increasing pressure of absorption in the spectral range containing the ν2 band. This result is attributed to the Coriolis coupling between the ν2 and ν4 vibrational states and to a contribution whose physical origin remains unclear. The latter, which is negligible when CH4–He mixtures are considered, behaves as collision-induced absorption. © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.1289243
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  • 6
    Electronic Resource
    Electronic Resource
    A molecular beam/surface spectroscopy apparatus for the study of reactions on complex model catalysts (2000)
    [S.l.] : American Institute of Physics (AIP)
    Review of Scientific Instruments 71 (2000), S. 4395-4408 
    Details
    ISSN: 1089-7623
    Source: AIP Digital Archive
    Topics: Physics , Electrical Engineering, Measurement and Control Technology
    Notes: We describe a newly developed ultrahigh vacuum (UHV) experiment which combines molecular beam techniques and in situ surface spectroscopy. It has been specifically designed to study the reaction kinetics and dynamics on complex model catalysts. The UHV system contains: (a) a preparation compartment providing the experimental techniques which are required to prepare and characterize single-crystal based model catalysts such as ordered oxide surfaces or oxide supported metal particles; and (b) the actual scattering chamber, where up to three molecular beams can be crossed on the sample surface. Two beams are produced by newly developed differentially pumped sources based on multichannel arrays. The latter are capable of providing high intensity and purity beams and can be modulated by means of a vacuum-motor driven and computer-controlled chopper. The third beam is generated in a continuous or pulsed supersonic expansion and is modulated via a variable duty-cycle chopper. Angular and time-resolved measurements of desorbing and scattered molecules are performed with a rotatable doubly differentially pumped quadrupole mass spectrometer with a liquid-nitrogen cooled ionizer housing. Time-resolved but angle-integrated measurements are realized with a second nondifferentially pumped quadrupole mass spectrometer. In situ measurements of adsorbed species under reaction conditions are performed by means of an adapted vacuum Fourier transform infrared spectrometer. The spectrometer provides the possibility of time-resolved measurements and can be synchronized with any of the beam sources. This contribution provides a general overview of the system and a description of all new components and their interplay. We also present test data for all components employing simple adsorption/desorption and reaction systems. © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.1318919
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  • 7
    Electronic Resource
    Electronic Resource
    X-ray standing wave study of MnTe fractional monolayers inserted in CdTe (001) (2000)
    [S.l.] : American Institute of Physics (AIP)
    Journal of Applied Physics 88 (2000), S. 4889-4897 
    Details
    ISSN: 1089-7550
    Source: AIP Digital Archive
    Topics: Physics
    Notes: The x-ray standing wave method is used in correlation with reflection high-energy electron diffraction and scanning tunneling microscopy to investigate the crystallographic features of MnTe monolayers inserted in CdTe (001). Either conventional molecular beam epitaxy or atomic layer epitaxy were employed for the formation of the CdTe starting surface, the deposition of the MnTe fractional monolayer, and its encapsulation by CdTe. Significant differences concerning the ratio of Mn atoms involved in MnTe clusters to those incorporated as part of a CdMnTe alloy are observed between the samples. Those differences are due to differing CdTe starting surface roughness. © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.1311829
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  • 8
    Electronic Resource
    Electronic Resource
    Interface dilution and morphology of CdTe/MnTe superlattices studied by small- and large-angle x-ray scattering (2000)
    [S.l.] : American Institute of Physics (AIP)
    Journal of Applied Physics 87 (2000), S. 7266-7274 
    Details
    ISSN: 1089-7550
    Source: AIP Digital Archive
    Topics: Physics
    Notes: We have performed small- and large-angle x-ray scattering experiments on CdTe/MnTe superlattices. The Fresnel optical method and the distorted wave Born approximation were used to extract from small-angle measurements out-of-plane and in-plane information about the interfaces. Specular reflectivity shows that the interface roughness is quite high (about 7 Å) for all superlattices. The effective MnTe concentration, directly determined from the refractive index profile, is successfully used to simulate the structured nonspecular scattering, and to determine the lateral correlation length of the interface roughness (about 1500±750 Å). Moreover, it is shown that the layers are almost completely correlated over the sample thickness. The thickness fluctuations along the growth direction are estimated from the analysis of the large-angle (004) reflection, and the effective MnTe profile is also checked by dynamical simulation. It is shown that the small- and large-angle results are in good agreement. The MnTe profile width deduced from x-ray reflectivity is slightly overestimated due to the large integration area of this technique. An estimation of the local MnTe profile is given. © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.372979
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  • 9
    Electronic Resource
    Electronic Resource
    IR absorption of highly vibrationally excited SF6 (1978)
    Springer
    Applied physics 15 (1978), S. 297-301 
    Details
    ISSN: 1432-0630
    Keywords: 33
    Source: Springer Online Journal Archives 1860-2000
    Topics: Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics , Physics
    Notes: Abstract In a double-resonance experiment, the absorption of various CO2 laser lines by sulfur hexafluoride was measured, before and after the SF6 was pumped by a fixed frequency CO2 laser to a level of 5 quanta/molecule. The absorption is substantially shifted to longer wavelengths. But the short wavelength wing of the absorption band is not completely bleached. Instead a shoulder of several cm−1 width is left. This shoulder is probably important for the explanation of the infrared laser induced dissociation of SF6.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1007/BF00896111
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  • 10
    Electronic Resource
    Electronic Resource
    Technische Thermodynanzik in Beispielen. Teil 1 : Grundlagen. Von J. U. KELLER. Berlin/New York: Walter de Gruyter 1979. XV, 307 S., flexibler Einband, DM 39. - . (1979)
    Weinheim : Wiley-Blackwell
    Acta Polymerica 30 (1979), S. 528-528 
    Details
    ISSN: 0323-7648
    Keywords: Chemistry ; Polymer and Materials Science
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology , Physics
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/actp.1979.010300816
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