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  • American Institute of Physics (AIP)  (478)
  • American Meteorological Society (AMS)
  • 1
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 112 (2000), S. 3345-3350 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Canonical ensemble molecular dynamics simulations were conducted for methane diffusion in AlPO4-5 in order to assess the role of the lattice motion on adsorbate diffusivity in straight pore zeolites. Both a static lattice model and a full dynamic lattice model were used at a loading of 1.5 methane/unit cell at 295 K. Although recent simulation work has asserted that there should be a difference, we show that there is little difference in the observed methane diffusivity (1.26×10−7 m2/s) and passing frequency (0.305) when a static lattice approximation is used over a full dynamic lattice (1.33×10−7 m2/s and 0.328). Furthermore, we introduce a methodology for handling lattice motion in molecular simulations by utilizing the normal vibrational modes in a harmonic crystal approximation. © 2000 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 111 (1999), S. 859-874 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Many systems approach equilibrium slowly along surfaces of dimension smaller than the original dimensionality. Such systems include coupled chemical kinetics and master equations. In the past the steady state approximation has been used to estimate these lower dimensional surfaces, commonly referred to as "manifolds," and thus reduce the dimensionality of the system which needs to be studied. However, the steady state approximation is often inaccurate and sometimes difficult to define unambiguously. In recent years two methods have been proposed to go beyond the steady state approximation to improve the accuracy of dimension reduction. We investigate these methods and suggest significant modifications to one of them to allow it to be used for the generation of low-dimensional manifolds in large systems. Based on the geometric investigations, two other approaches are suggested which have some advantages over these two methods for the cases studied here. All four approaches are geometric and offer advantages over methods based on the evaluation of time-dependent behavior, where phenomenological rate laws are extracted from the time-dependent behavior. © 1999 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 109 (1998), S. 7793-7802 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: High-resolution infrared spectra of jet-cooled allyl (CH2–CH–CH2) radical in the CH2 stretching region are obtained in a slit jet discharge spectrometer. Over 200 transitions are observed in the 3100–3140 cm−1 region, which have been rigorously assigned to "in-phase" (ν1) and "out-of-phase" (ν13) coupling of antisymmetric CH stretch excitations on each of the equivalent CH2 subunits. Origins for the two bands are determined to be 3113.98 488(89) cm−1 (ν1) and 3110.59 857(36) cm−1 (ν13), respectively. The data are reasonably well fit to semirigid asymmetric rotor behavior for the Ka≤2 levels populated in the slit jet at Trot(approximate)20 K, though not to within the experimental precision, which provides some indication of perturbations in the upper states. The sign and magnitude of the +3.4 cm−1 splitting between"in-phase" and"out-of-phase" excitations are in good qualitative agreement with a simple electrostatic model of dipole–dipole coupling between the two "local mode" CH2 groups. Due to sub-Doppler resolution (Δν(approximate)70 MHz) in the slit jet expansion, quantum-state-dependent excess broadening of the rovibrational transitions is observed, which can be ascribed to spin–rotation interactions. Based on a least squares analysis of the high-resolution line shapes, the data are consistent with a spin rotation constant of cursive-epsilonaa(approximate)−67(25) MHz. © 1998 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 107 (1997), S. 943-952 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The initial dissociative chemisorption probability, S0, of O2 on Ir(111) has been investigated with molecular beam techniques and electron energy loss spectroscopy (EELS). The adsorption process on the clean surface occurs by distinct dynamical mechanisms. At incident kinetic energies, Ei, of 0.1 eV and below, the dissociative chemisorption probability decreases with increasing kinetic energy, indicating the dominance of a trapping-mediated mechanism. A decrease in the value of S0 with increasing surface temperature, Ts, is also characteristic of this regime. This temperature dependence reflects the participation of a physically adsorbed state and molecularly chemisorbed state in the dissociation scheme. Additionally, the dependence of S0 on incident angle, θi, in the low kinetic energy regime exhibits near normal energy scaling. At high kinetic energy (Ei〉0.1 eV), the initial dissociative chemisorption probability rises with increasing Ei indicating that translational energy is effective in surmounting a potential barrier to adsorption. Direct access of a molecularly chemisorbed state followed by dissociation, rather than direct access of the dissociated state, is hypothesized to be the primary initial adsorption step. Several observations support this mechanism, including a temperature dependence in the high kinetic energy regime and no observed increase in oxygen saturation coverage with increasing kinetic energy. In addition, EEL spectra show that molecularly chemisorbed states of oxygen are formed on the Ir(111) surface at Ts〈70 K after exposure to a 1.36 eV beam and partial saturation of the atomic overlayer. Attempts to identify molecularly chemisorbed oxygen at low coverages were unsuccessful and limited by the experimental setup which provides cooling of the iridium crystal to only ∼68 K. © 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 107 (1997), S. 5661-5675 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A novel high-intensity source of jet-cooled molecular radicals is described based on the combination of (i) slit supersonic expansions with (ii) pulsed electric discharges. The electrode bias configuration effectively confines the discharge to a region upstream of the supersonic expansion, which results both in efficient rotational cooling (Trot(approximate)25 K) and high radical densities (〉1014/cm3). In conjunction with direct absorption laser probe methods, this discharge source provides a general technique for high-resolution IR studies of jet-cooled radicals. Performance of the slit discharge system is demonstrated on v=1←0 rovibrational transitions in jet-cooled OH radicals, which indicate sub-Doppler linewidths (Δν(approximate)100 MHz) when probed along the slit expansion axis. The enhanced spectral resolution of the slit discharge geometry is utilized to probe the v3=1←0 asymmetric CH stretch vibration–rotation spectra of CH3 radical. Under sub-Doppler conditions, spin–rotation splittings are fully resolved and nuclear hyperfine splittings partially resolved in all of the transitions, permitting the first measure of Fermi contact interactions [af″=−65.5(9) MHz, εbb″=−354(5) MHz, af′=−65(2) MHz, εbb′=−353(2) MHz] and therefore both the sign and magnitude of spin-polarization effects for CH3 under isolated gas-phase conditions. The results permit direct comparison with high level ab initio calculations, and highlight a clear trend in spin-polarization effects between condensed and gas-phase behavior. © 1997 American Institute of Physics.
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  • 6
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Journal of Applied Physics 80 (1996), S. 2873-2882 
    ISSN: 1089-7550
    Source: AIP Digital Archive
    Topics: Physics
    Notes: Cadmium sulfide (CdS) layers were deposited from an aqueous solution of thiourea, cadmium sulfate, and ammonia on (100) n-InP at 60–95 °C. X-ray photoelectron spectroscopy showed that the deposition process effectively removes native oxides on InP and forms a protective layer for subsequent dielectric deposition. Surface analysis also showed that the InP surface is not P deficient following oxide deposition on CdS-treated InP. Capacitance–voltage and conductance–voltage measurements of metal–insulator–semiconductor (MIS) capacitors were used to compare samples with and without CdS films between InP and a deposited insulator. Capacitance–voltage response of CdS-treated MIS structures showed well-defined regions of accumulation, depletion, and inversion. The interface-state density at midgap was reduced from 5×1011 to 6×1010 eV−1 cm−2 with CdS treatment. Depletion-mode MIS field-effect transistors made using this new passivation technique exhibited superior device performance to that of untreated samples.
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  • 7
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Journal of Applied Physics 79 (1996), S. 2863-2867 
    ISSN: 1089-7550
    Source: AIP Digital Archive
    Topics: Physics
    Notes: Multiple energy He+ ion implantation to increase the width of the implantation-induced refraction index barrier in LiB3O5 (LBO) is reported. Improvements in planar waveguide transmission (coupling and propagation) at the HeNe laser wavelength of 633 nm, from 5% to 45% for TE polarized light, and from 10% to 28% for TM polarized light in a ∼5-mm-long LBO planar waveguide are shown. Annealing is found to increase the transmission (coupling and propagation) at the wavelength of 633 nm of multiple-energy implanted planar LBO waveguides by as much as 24% for TE polarized light and 71% for TM polarized light. Channel waveguides in LBO fabricated by multiple-energy ion implantation through a gold wire mask and their use for second-harmonic generation are reported. © 1996 American Institute of Physics.
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  • 8
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Journal of Applied Physics 77 (1995), S. 5736-5738 
    ISSN: 1089-7550
    Source: AIP Digital Archive
    Topics: Physics
    Notes: We have studied the deep levels in the lattice-matched InP/(InAlGa)As heterojunction system. Five p-n junction samples were grown by metalorganic chemical vapor deposition with varied Al composition of 0%, 16%, 36%, 45%, and 55%. A vacancy-related deep electron trap was found at the InP/(InAlGa)As interface. This trap has less concentration in the sample with higher Al composition, and is not observed when Al composition is greater than 55%. Its activation energy within the band gap increases with the increasing Al composition. The trap can be eliminated by rapid thermal annealing at 700 °C. Current-voltage characteristics show that this trap acts as recombination centers under forward bias condition. © 1995 American Institute of Physics.
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  • 9
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Journal of Applied Physics 79 (1996), S. 3793-3795 
    ISSN: 1089-7550
    Source: AIP Digital Archive
    Topics: Physics
    Notes: The effect of applying an electric field across a quasi-phase-matched frequency doubling lithium tantalate waveguide has been investigated. The waveguide was fabricated by a two-stage ion exchange process in pyrophosphoric acid. An electric field of 2 kV/mm was found to shift the phase matching wavelength by 0.05 nm. It is estimated that more optimized waveguides could produce wavelength shifts of ±4 nm for an applied electric field of ±20 kV/mm and could compensate for temperature variations of ±67 °C. © 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. 2237-2244 
    ISSN: 1089-7550
    Source: AIP Digital Archive
    Topics: Physics
    Notes: The plasma characteristics of a new arc mode on carbon referred to as the "stationary cathodic arc'' are reported. Particularly, optical emission spectroscopy, probe and ion energy distribution measurements are used to compare the properties of the stationary arc with the normal "random cathodic arc'' on carbon. The measurements revealed that the plasma properties of both arc modes are similar. In addition, we have correlated the plasma characteristics to the film properties. Carbon films deposited using the stationary arc were found to have a surface particle density equivalent to those deposited using the filtered cathodic vacuum arc. The macro-particle free films were found to be highly tetrahedral and compressively stressed. Both the sp3 fraction and stress values were strongly dependent on the ion energy with maximum values of 85% and 9.4 GPa, respectively, occurring at ≈50 eV. © 1996 American Institute of Physics.
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