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  • 11
    ISSN: 1089-7550
    Source: AIP Digital Archive
    Topics: Physics
    Notes: Epitaxial PbTiO3 films were prepared by metalorganic chemical-vapor deposition on MgO(001)-, SrTiO3(001)-, and LaAlO3(001)-oriented substrates. Four-circle x-ray diffraction, transmission electron microscopy, Rutherford backscattering (RBS) channeling, and optical waveguiding were performed to characterize the deposited films. Epitaxial, single-crystal films were obtained on all three substrate materials under the same growth conditions. However, the defect structure of the films, including grain tilting, threading dislocation density, and 90° domain formation, was strongly dependent on the choice of substrate material. Films grown on MgO(001) and LaAlO3(001) (pseudocubic indices) substrates are nominally c-axis oriented; however, the PbTiO3 grains in the film form a fourfold domain structure, with the grains tilted ∼0.6° and ∼0.7°, respectively, toward the [100] directions (cubic or pseudo-cubic) of the substrates. In addition, these films contain a significant volume fraction of 90°-domain (a-axis) structures with a critical thickness hc for domain formation below the detection level of our experiments (hc≥100 A(ring)). Together, these structural defects result in a low RBS channeling yield reduction. In contrast, films grown on SrTiO3(001) substrates showed no tilting of the c-axis grains and a minimum RBS channeling yield of as low as ∼3%. In addition, we observed that below a critical film thickness of hc∼1500 A(ring), 90° domain formation was completely suppressed resulting in a nearly perfect single-crystal structure.The refractive indices and optical birefringence of the films were measured as a function of wavelength using the film-prism coupling method. Both the ordinary and extraordinary refractive indices for films grown on MgO(001) and LaAlO3(001) were higher than that of single-crystal PbTiO3; however, the optical birefringence of films grown on MgO(001) was reduced from that of the bulk. For films grown on SrTiO3(001), the ordinary refractive index was very close to that of single-crystal PbTiO3. We correlate the refractive index values and the reduced birefringence to the degree of residual strain and the volume fraction of 90° domains in the samples, respectively. © 1995 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 12
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 109 (1998), S. 10082-10086 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We study a soliton-like distortion in a quasi-one-dimensional conjugated carbon chain with a single side radical, which contains an unpaired electron, by taking into account the electron–phonon interaction, an extended Hubbard term due to on-site electron–electron interactions and intersite e–e interactions, and the ferromagnetic correlation between itinerant π-electrons and the unpaired radical electron. It is shown that a critical value of hopping integral exists between the side radical and the main chain, at which a transition from a single soliton-like distorted structure to a pair of soliton-like distortions occurs along the main chain. In addition, the spin density at the dangling site is transferred to the main chain due to the hopping interaction between the main chain and the side radical, and the spin density at the side radical is decreased to zero when the hopping integral is larger than the critical value. © 1998 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 13
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 107 (1997), S. 1544-1550 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Molecular dynamics simulations based on pseudopotentials are used to characterize the difference between impurity rotations in classical versus quantum solids. The method is first applied to the pure solids and demonstrated to faithfully reproduce static and dynamical properties, in the form of pair distributions and phonon density of states of solid H2(D2). Then the rotations of molecular oxygen in the ground X(3Σg−) and electronically excited state A(3Δu) is investigated. Where the substitutional impurity is small, O2(X), in the classical solid, the cavity remains nearly spherical and the molecule undergoes rotation-translation coupled motion. In contrast, in the quantum solid, the lattice locally distorts around the impurity and forces librations with occasional reorientational hops as rotation-distortion coupled motion. These effects are amplified in the excited O2(A) state, in which due to the larger molecular bond length, the angular anisotropy of the guest–host interaction is larger. Now, in the classical solid a small cage distortion forces the molecule into large amplitude librations. The molecule, however, reorients occasionally, when the lattice fluctuations lead to a nearly spherical cage geometry. In the quantum host, O2(A) becomes a strict librator, due to a large and permanent deformation of the soft cage. The results are used to rationalize experimental observations. © 1997 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 14
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 109 (1998), S. 134-138 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The equilibrium structures and harmonic vibrational frequencies for CHBr+, CBr+, and their neutrals have been determined using second-order Møller–Plesset perturbation theory, singles and doubles configuration interaction theory, and coupled-cluster theory in conjunction with the triple-zeta double-polarized and 6-311++G(3df,3pd) basis sets. The coupled-cluster results are in good agreement, for the experimental geometries and harmonic frequencies, with available experimental data. The adiabatic ionization potentials are predicted to be 205.7 kcal mol−1 for CHBr and 197.5 kcal mol−1 for CBr. © 1998 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 15
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 101 (1994), S. 6648-6657 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The caging of I2 in solid Kr is followed in real-time following its dissociative excitation on the A(3Π1u) surface. The experiments involve pump–probe measurements with a time resolution of ≥150 fs. The experimental signals are reproduced using classical molecular dynamics simulations, and the classical Franck approximation. The comparison between experiment and simulation allows an unambiguous interpretation of features in the observed signal as being due to the initial impulsive stretch of the I–I bond, collision of the atoms with the cage wall, recoil and recombination, and the subsequent coherent oscillations of the nascent I2 molecule. These detailed observations are possible due to retention of coherence along the I–I coordinate throughout the caging process. The extent of coherence is dictated mainly by the initial impact parameters of the molecule-cage collision, which in turn is controlled by the thermal and zero-point amplitudes of lattice vibrations. The caging is well-described as a sudden process, involving a binary collision between I and Kr atoms with nearly complete energy loss of the I atom upon completion of the first collision. Vibrational relaxation of the bound molecule proceeds on the time scale of 12 ps. The nontrivial relation between this relaxation time and decay rates that may be extracted from experimental transients is discussed. Although the interplay between the nested A and A' potentials is not detectable, it is clear that in the studied range of initial excess energies, 1000–1700 cm−1, the recombination remains effectively adiabatic, and does not involve the ground state.
    Type of Medium: Electronic Resource
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  • 16
    Electronic Resource
    Electronic Resource
    s.l. : American Chemical Society
    Langmuir 10 (1994), S. 330-333 
    ISSN: 1520-5827
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology
    Type of Medium: Electronic Resource
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  • 17
    ISSN: 1520-5827
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology
    Type of Medium: Electronic Resource
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  • 18
    ISSN: 1520-5827
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology
    Type of Medium: Electronic Resource
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  • 19
    ISSN: 1520-5827
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology
    Type of Medium: Electronic Resource
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  • 20
    Electronic Resource
    Electronic Resource
    s.l. : American Chemical Society
    Macromolecules 22 (1989), S. 4273-4277 
    ISSN: 1520-5835
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology , Physics
    Type of Medium: Electronic Resource
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