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  • Springer  (30)
  • American Institute of Physics (AIP)  (15)
  • 2010-2014  (8)
  • 2000-2004  (8)
  • 1985-1989  (29)
  • 1
    Digitale Medien
    Digitale Medien
    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
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: 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.
    Materialart: Digitale Medien
    URL: http://dx.doi.org/10.1063/1.480597
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  • 2
    Digitale Medien
    Digitale Medien
    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
    Quelle: AIP Digital Archive
    Thema: Physik , Elektrotechnik, Elektronik, Nachrichtentechnik
    Notizen: 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.
    Materialart: Digitale Medien
    URL: http://dx.doi.org/10.1063/1.1318919
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  • 3
    Digitale Medien
    Digitale Medien
    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
    Quelle: AIP Digital Archive
    Thema: Physik
    Notizen: 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.
    Materialart: Digitale Medien
    URL: http://dx.doi.org/10.1063/1.372979
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  • 4
    Digitale Medien
    Digitale Medien
    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
    Quelle: AIP Digital Archive
    Thema: Physik
    Notizen: 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.
    Materialart: Digitale Medien
    URL: http://dx.doi.org/10.1063/1.1311829
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  • 5
    Digitale Medien
    Digitale Medien
    Collisional broadening of CO2 IR lines. II. Calculations (1988)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 88 (1988), S. 2999-3006 
    Details
    ISSN: 1089-7690
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: The ability of available theoretical models in describing broadening mechanisms is tested for the CO2–O2, CO2–CO2, and CO2–N2 systems. It is shown that the Anderson–Tsao–Curnutte theory is inaccurate since short-range forces can contribute significantly to broadening. We use the approach of Robert and Bonamy, but the usual expansion of the atom–atom potential to the fourth order around the intermolecular distance appears insufficient at short distances for these particular systems. We propose a better representation of the radial dependence of the atom–atom potential, while keeping the previous analytical expression of the cross section. Satisfactory results are obtained for both the rotational quantum number dependence of room-temperature CO2–O2, CO2–CO2, and CO2–N2 half-widths and the evolution of CO2–N2 broadening with temperature. It is shown that the isotropic part of the potential involved in the trajectory calculation must be coherently deduced from the atom–atom interaction potential.
    Materialart: Digitale Medien
    URL: http://dx.doi.org/10.1063/1.453941
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  • 6
    Digitale Medien
    Digitale Medien
    Collisional broadening of rotation–vibration lines for asymmetric-top molecules. II. H2O diode laser measurements in the 400–900 K range; calculations in the 300–2000 K range (1987)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 86 (1987), S. 144-156 
    Details
    ISSN: 1089-7690
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: Numerous comparisons between predictions of the model presented in part I of this paper and experimental H2O infrared linewidths are presented. It is shown that our model, contrary to those used up to now, gives accurate results for H2O room-temperature line broadening by O2 and Ar, and for high rotational quantum-number lines by N2. First accurate experimental widths and intensities of some H2O ν2-band lines in the 400–900 K temperature range are also presented. Detailed analysis of the data demonstrates the great influence of a "resonance overtaking'' mechanism. The latter results from the modifications of both the perturber rovibrational population distribution and kinetic energy with temperature; it strongly enhances the contributions of the collision-induced rotational transitions involving significant energy jumps. This mechanism is well accounted for by our model and quantitatively explains the unusually slow decrease of some linewidths with temperature.
    Materialart: Digitale Medien
    URL: http://dx.doi.org/10.1063/1.452605
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  • 7
    Digitale Medien
    Digitale Medien
    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
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: 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.
    Materialart: Digitale Medien
    URL: http://dx.doi.org/10.1063/1.1424311
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  • 8
    Digitale Medien
    Digitale Medien
    Collisional broadening of rotation–vibration lines for asymmetric top molecules. I. Theoretical model for both distant and close collisions (1986)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 84 (1986), S. 4256-4267 
    Details
    ISSN: 1089-7690
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: A semiclassical theory of infrared linewidths in the gas, previously developed for linear molecules, is extended to asymmetric top molecules. It includes a satisfactory treatment of the close collisions and is consequently adapted to describe the temperature dependence of the linewidths, in particular in the combustion temperature range. Numerical applications to the water vapor perturbed by nitrogen, oxygen, and argon show strong different behaviors following the nature of the perturber. For oxygen and argon perturbers, the contribution of close collisions is the predominant mechanism of line broadening. The consistency of the theoretical model is evidenced by comparison with precise measurements for H2O–N2, –O2, and Ar at 300 K. Moreover, the calculated temperature dependence of the linewidths is compared with recent experimental data for H2O–Ar between 1300 and 2300 K.
    Materialart: Digitale Medien
    URL: http://dx.doi.org/10.1063/1.450047
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  • 9
    Digitale Medien
    Digitale Medien
    Line broadening, line shifting, and line coupling effects on N2–H2O stimulated Raman spectra (1989)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 91 (1989), S. 5916-5925 
    Details
    ISSN: 1089-7690
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: In order to understand the influence of H2O on the stimulated Raman Q-branch spectra of nitrogen in combusting media, an exhaustive theoretical and experimental study has been carried out. Starting from a semiclassical model, particularly convenient at high temperature, the Q-line broadening and shifting coefficients have been calculated over a wide temperature range and for a large number of lines. Stimulated Raman Spectra (SRS) measurements have allowed us to test these calculated line broadening coefficients and thus establish the high accuracy of semiclassical values. The theoretical broadening coefficients have been inverted to deduce state-to-state rotational relaxation rates by using two types of fitting laws. A partial test of the resulting Q-branch profiles has been realized at moderate pressures leading to a discrimination between these two laws. Furthermore, the effect of rotational energy transfers on collisionally narrowed profiles at higher densities has been simulated and compared with the pure N2 case.
    Materialart: Digitale Medien
    URL: http://dx.doi.org/10.1063/1.457461
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  • 10
    Digitale Medien
    Digitale Medien
    Measurements and calculations of CO2 room-temperature high-pressure spectra in the 4.3 μm region (1989)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 90 (1989), S. 2944-2950 
    Details
    ISSN: 1089-7690
    Quelle: AIP Digital Archive
    Thema: Physik , Chemie und Pharmazie
    Notizen: Measurements of the absorption by pure CO2 in the 4.3 μm region are presented. They refer to the temperature of 291 K and densities in the 1–80 amagat range. Calculations based on the addition of Lorentzian contributions strongly overestimate the absorption since they do not account for line overlapping. The energy corrected sudden approximation (ECSA) is used to model line mixing within the impact approximation. The scaling parameters of this model are deduced from line-broadening data. This calculation strongly underestimates the absorption in the spectral region near the edges of the vibrational band, whereas it overestimates the absorption in the far wings of the lines. This is attributed to the impact approximation which does not account for the frequency dependence of the relaxation operator. This dependence is roughly determined from our results; it is in good qualitative agreement with the few corresponding available results.
    Materialart: Digitale Medien
    URL: http://dx.doi.org/10.1063/1.455894
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