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  • 1
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Journal of Applied Physics 73 (1993), S. 1737-1742 
    ISSN: 1089-7550
    Source: AIP Digital Archive
    Topics: Physics
    Notes: In situ Si-TaSi2 composites are studied by synchrotron white beam topography and by double axis diffractometry. These results show that the single crystal Si matrix is of excellent quality: Rocking curve widths are between 40 and 60 s of arc, and the topographs do not exhibit asterism. Diffuse radial streaks in the Laue patterns originate from diffraction by the TaSi2 rods in the matrix: The K-absorption edge of filters placed in the incident x-ray beam produces a sharp change in contrast in the streaks, and this is used to determine the d spacings present in the streaks and to show that considerable preferred orientation exists between the TaSi2 rods and the Si matrix.
    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 96 (1992), S. 5298-5309 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Potential-energy functions of the three lowest singlet states of pyrazine have been computed on the self-consistent field, second-order Møller–Plesset (SCF/MP2) level as a function of ab initio determined ground-state normal coordinates. The electronic-structure calculations confirm the existence of a conical intersection of the S1(nπ*) and S2(ππ*) surfaces near the minimum of the latter surface. A vibronic-coupling model involving four spectroscopically active vibrational modes is constructed on the basis of the ab initio data. Absorption, resonance-Raman, fluorescence, and femtosecond time-resolved pump–probe spectra are computed for this model using previously developed methods. The results are compared with experimental data where available.
    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 93 (1990), S. 5496-5509 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A theoretical description of secondary emission from complex absorption bands of isolated polyatomic molecules is developed. The strong non-Born–Oppenheimer coupling associated with conical intersections of the multidimensional excited-state potential-energy surfaces is included in a fully microscopic manner by solving the time-dependent Schrödinger equation for appropriate model systems incorporating the most relevant electronic states and vibrational modes. The effect of the large number of remaining vibrational modes and of the weaker coupling with additional electronic states is modeled by phenomenological relaxation terms (lifetime broadening and pure dephasing) in the framework of the density-matrix formalism. Explicit eigenstate-free expressions for absorption, resonance Raman, and fluorescence spectra are derived via density-matrix perturbation theory. The computational feasibility of the resulting mixed microscopic/phenomenological theory is demonstrated for a simple three-mode model of the vibronic coupling of the S1(nπ*) and S2(ππ*) states of pyrazine. The effect of excited-state vibronic coupling and ultrafast S2→S1 internal conversion on resonance Raman and fluorescence spectra is analyzed on the basis of these model calculations.
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  • 4
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 90 (1989), S. 7184-7194 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We present a computer simulation of the real-time detection of ultrafast electronic decay dynamics in polyatomic molecules with femtosecond laser pulses. The intramolecular non-Born-Oppenheimer quantum dynamics is treated numerically exactly for a two-state three-mode vibronic coupling model representing the conically intersecting S1 and S2 excited states of pyrazine. The pump–probe signal is evaluated in lowest order perturbation theory with respect to the radiation–matter interaction by numerical integration over the pump and probe pulses. We discuss in some detail the dependence of the pump–probe signal on the properties of the laser pulses (frequencies and pulse durations). The calculations predict a dramatic (∼12 000 cm−1) and ultrafast (∼20 fs) red shift of the stimulated-emission signal as well as distinctive quantum beats in the pump–probe signal as a function of the delay time. Both effects are very pronounced and should therefore be relatively easily detectable experimentally. They are expected to be generic features of ultrafast internal-conversion processes in polyatomic molecules.
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  • 5
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 99 (1993), S. 1545-1555 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A general classical formulation of the spectroscopy of nonadiabatically coupled electronic states is developed within the theoretical framework of the classical electron analog model due to Meyer and Miller. Adopting the Heisenberg representation for the calculation of the electric polarization, several approaches are presented to establish a quantum-classical correspondence. It is shown that a consistent classical formulation is obtained by replacing the quantum-mechanical commutators, which appear in quantum-mechanical perturbation theory, by the corresponding classical Poisson brackets which come from classical perturbation theory. The more usual practice of replacing the Heisenberg dipole operators directly by the corresponding classical dipole functions is shown to be an approximation to classical perturbation theory. For a coupled electronic three-state system explicit expressions are derived for the nonlinear polarization. Furthermore the practical application to femtosecond pump-probe spectroscopy is discussed in some detail.
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  • 6
    ISSN: 1089-7623
    Source: AIP Digital Archive
    Topics: Physics , Electrical Engineering, Measurement and Control Technology
    Notes: The wide matrix rocking curves of the in situ eutectic composite TaSi2-Si make it attractive as a wide-bandpass monochromator for synchrotron radiation. Wafers with Si[111], Si[110], or Si[100] orientation were studied to determine the origin of the wide rocking curves. The high degree of preferred orientation of the TaSi2 rods relative to the Si matrix was examined using synchrotron Laue patterns and the TaSi2 [100], TaSi2 [003], and TaSi2 [102] reflections. Double and triple axis diffractometry were used to show that the large widths were due to strain and mosaic and not long-range bending; copper radiation (for some double axis results) and 120 and 160 keV synchrotron radiation were used. At 8 keV, rocking curve widths were about twenty times broader than those from perfect Si, and peak reflectivities approached 20%. Rocking curves from Si[333] and Si[444] (120 and 160 keV, respectively) had identical profiles and reflectivities of about 25%. The triple axis results show compressive strains in the Si matrix along Si[111] (i.e., parallel to the rods) and dilational strains orthogonal to the rods. These results confirm the promise of TaSi2-Si as a wide-bandpass optical element for synchrotron radiation. © 1996 American Institute of Physics.
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  • 7
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Review of Scientific Instruments 66 (1995), S. 28-31 
    ISSN: 1089-7623
    Source: AIP Digital Archive
    Topics: Physics , Electrical Engineering, Measurement and Control Technology
    Notes: A target of gaseous polarized hydrogen was formed by injecting polarized hydrogen atoms (produced by Stern–Gerlach spin separation) into a storage cell consisting of a cylindrical tube open at both ends. The target was placed in a storage ring to study the target characteristics (nuclear polarization, target thickness, radiation resistance). A weak transverse guide field (5 G) was applied to define the polarization direction. When atoms in a single hyperfine state were selected, the nuclear polarization of the target was measured to be 0.80±0.02. The areal density of the target under these conditions was (5.5±0.2)×1013 H/cm2, while for two spin states (applicable to experiments in high energy rings where a strong magnetic field can be applied to the target) the target thickness was found to be (8.2±0.3)×1013 H/cm2. The target polarization was unaffected by prolonged exposure of the target to beams up to 1 mA. © 1995 American Institute of Physics.
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  • 8
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Review of Scientific Instruments 68 (1997), S. 1939-1944 
    ISSN: 1089-7623
    Source: AIP Digital Archive
    Topics: Physics , Electrical Engineering, Measurement and Control Technology
    Notes: A W/Si multilayer was used to determine the degree of circular polarization of the soft x-ray radiation of the European Synchrotron Radiation Facility helical undulator HELIOS I. The multilayer, manufactured by vapor deposition serves as a wideband tunable polarization analyzer in the photon energy range from 520 to 930 eV. The characterization of the multilayer's analyzing power, varying from 0.82 to 0.25 for these energies, indicates that it operates close to its calculated specifications. The lack of phase-shifters applicable in this energy range was overcome by a detailed analysis of the unpolarized background identified as radiation from the magnetic lattice. In this way, the degree of circular polarization of HELIOS I was determined to exceed 0.85 for hν〉685 eV. © 1997 American Institute of Physics.
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  • 9
    ISSN: 1089-7623
    Source: AIP Digital Archive
    Topics: Physics , Electrical Engineering, Measurement and Control Technology
    Notes: In understanding the macroscopic response of polycrystalline structural materials to loading, it is frequently essential to know both the three-dimensional distribution of strain and of microtexture. The methods must be nondestructive, however, if the evolution of quantities, such as strain at a fatigue crack tip, are to be studied. This paper describes approaches for high resolution synchrotron x-ray diffraction tomography of polycrystalline materials. Preliminary experiments are reported on partially cracked compact tension samples of Al-Li 2090 and on model samples of randomly packed, millimeter-sized single crystals. Polychromatic beams collimated to diameters as small as 30 μm have been used, and collecting the spatial distribution of diffracted intensity on image storage plates as a function of sample-to-detector separation allowed inference of the depth of the volume elements contributing to diffraction. The precision to which one can determine the depths of volume elements will be discussed as well approaches for three-dimensional, nondestructive strain mapping. © 1996 American Institute of Physics.
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  • 10
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Journal of Applied Physics 79 (1996), S. 6803-6810 
    ISSN: 1089-7550
    Source: AIP Digital Archive
    Topics: Physics
    Notes: The wide rocking curves of matrix reflections of the in situ eutectic composite TaSi2–Si make wafers of this material attractive for use as wide-bandpass monochromators for synchrotron radiation, and characterization of wafers of TaSi2–Si for use with energies normally accessible at storage rings (i.e., 5–40 keV) is the focus of the present report. A wafer with [111]Si orientation and a wafer with [110]Si orientation are studied. The high degree of preferred orientation of the TaSi2 rods relative to the Si matrix is examined using synchrotron Laue patterns, and the 100TaSi2, 003TaSi2, 101TaSi2, and 102TaSi2 reflections are used to establish the orientation relationship and to determine that the spread of rod orientations is at least 5° and probably no greater than 6°. Double-axis diffractometry with Cu Kα radiation reveals matrix reflections with rocking curve widths that are about 20 times broader than those from perfect Si and with peak reflectivities approaching 20%. The rocking curves widths are found to be relatively insensitive to irradiated area, thus indicating that most of the observed width is not due to long-range bending. Triple-axis diffractometry with Cu Kα radiation reveals that considerable compressive strain exists in the matrix and that much of the width of the diffraction peak is due to mosaicity. The performance of the [111]Si TaSi2–Si wafer and a perfect [111] Si wafer as monochromators for microradiography are compared, and a gain of an order of magnitude in x-ray intensity delivered to the sample is demonstrated with the composite crystal. © 1996 American Institute of Physics.
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