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  • 1
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 91 (1989), S. 711-721 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We have used ab initio methods to characterize the Ne–HF van der Waals complex. The interaction energy was determined using size consistent, correlated CEPA wave functions expanded in a Gaussian basis chosen to represent both intraatomic effects and the low order multipole moments and polarizabilities of Ne and HF. The calculated well depths are −65 cm−1 for linear Ne–HF and −39 cm−1 for linear Ne–FH, with an intervening saddle point at −27 cm−1. The induction contribution to the energy is significantly greater for Ne–HF than for Ne–FH, but dispersion remains the dominant attraction over the region of interest. Converged variational and close-coupling calculations using the ab initio potential surface reveal three bound levels of the Ne–HF stretch mode, and several metastable levels correlating asymptotically with rotationally excited HF( j=1). Though nearly degenerate, the lifetimes of the two metastable Π (body frame Λ=±1) bending levels differ markedly because of different rotational coupling strengths to the Σ (body frame Λ=0) bending state, which undergoes rapid rotational predissociation. From the calculated line positions, widths, and intensities we have synthesized far infrared and infrared spectra of Ne–HF and Ne–DF.
    Type of Medium: Electronic Resource
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  • 2
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: 294 transitions were measured by velocity modulation spectroscopy using a difference frequency laser system with a D2/O2 discharge and assigned to the ν3 (antisymmetric stretch) band of D3O+. A simultaneous analysis of this data with the ν2 band spectra reported by Sears, et al. [J. Chem. Phys. 83, 2676 (1985)] yielded a refined set of parameters for both the ground and the excited states of both bands. The ν3 bandcenters are 2629.6512(39) and 2624.2376(47) cm−1 for the s–s and a–a inversion components, respectively.
    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 91 (1989), S. 4418-4419 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The interconversion tunneling frequencies for (HCl)2 and (DCl)2 are obtained from near-infrared absorption spectra of the H(D)Cl stretching transitions, to spectroscopic precision for the mixed 35Cl–37Cl dimers. A phenomenological model of the interconversion process explains several experimental observations, and provides good estimates of the splittings expected for the 35Cl–35Cl and 37Cl–37Cl species.
    Type of Medium: Electronic Resource
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  • 4
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 91 (1989), S. 722-731 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Direct absorption tunable difference frequency IR spectroscopy in a slit jet supersonic expansion has been used to observe complexes of Ne with HF for the first time. Spectra of both the weak HF stretch fundamental (1000)←(0000) and the 10–20 fold more intense bend and stretch combination band (111e,f0)←(0000) transitions are observed, and illustrate several interesting dynamical features. The large ratio of combination band to fundamental intensity is evidence for a highly isotropic potential with respect to HF rotation. The HF bend vibration is thus better thought of as nearly free internal rotor motion with a nearly good space fixed quantum number, jHF =1. Weak anisotropy in the potential permits the jHF=1 (Πebend) levels to relax intramolecularly to jHF =0 (Σ) levels, leading to predissociative line broadening in the sub-Doppler slit jet spectra. This observed dissociation of NeHF with 44 cm−1 of internal excitation provides a rigorous upper limit to the binding energy. The Πfbend levels, on the other hand, have no lower energy internal rotor states of the correct parity to relax into, and thus the (111f0) ←(0000) spectra exhibit linewidths limited by the apparatus resolution. The internal relaxation of the jHF=1 (Πebend) levels results from Coriolis mixing with the Σbend states (1200) by overall rotation of the NeHF complex, and thus the lifetimes depend dramatically on J. The J-dependent predissociation rates observed are in remarkably quantitative agreement with quantum scattering calculations on the CEPA ab initio surface of ONeil and co-workers.
    Type of Medium: Electronic Resource
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  • 5
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 112 (2000), S. 3117-3120 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Single molecule confocal microscopy is used to study fluorescence intermittency of individual ZnS overcoated CdSe quantum dots (QDs) excited at 488 nm. The confocal apparatus permits the distribution of "on" and "off" times (i.e., periods of sustained fluorescence emission and darkness) to be measured over an unprecedentedly large dynamic range (109) of probability densities, with nonexponential behavior in τoff over a 105 range in time scales. In dramatic contrast, these same τoff distributions in all QDs are described with remarkable simplicity over this 109-fold dynamic range by a simple inverse power law, i.e., P(τoff)∝1/τoff1+α. Such inverse power law behavior is a clear signature of distributed kinetics, such as predicted for (i) an exponential distribution of trap depths or (ii) a distribution of tunneling distances between QD core/interface states. This has important statistical implications for all previous studies of fluorescence intermittency in semiconductor QDs and may have broader implications for other systems such as single polymer molecules. © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 6
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 115 (2001), S. 1028-1040 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Single molecule confocal microscopy is used to investigate the detailed kinetics of fluorescence intermittency in colloidal II–VI (CdSe) semiconductor quantum dots. Two distinct modes of behavior are observed corresponding to (i) sustained "on" episodes (τon) of rapid laser absorption/fluorescence cycling, followed by (ii) sustained "off" episodes (τoff) where essentially no light is emitted despite continuous laser excitation. Both on-time and off-time probability densities follow an inverse power law, P(τon/off)∝1/τon/offm, over more than seven decades in probability density and five decades in time. Such inverse power law behavior is an unambiguous signature of highly distributed kinetics with rates varying over 105-fold, in contrast with models for switching between "on" and "off" configurations of the system via single rate constant processes. The unprecedented dynamic range of the current data permits several kinetic models of fluorescence intermittency to be evaluated at the single molecule level and indicate the importance of fluctuations in the quantum dot environment. © 2001 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 7
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 114 (2001), S. 8596-8609 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The dramatic modifications of molecular fluorescence in the proximity of a sharp nanoscopic probe is investigated by an apertureless or antenna-based near-field scanning optical microscope, which exploits the interactions between a fluorescent sample and a laser illuminated Si atomic force microscope probe. Specifically, luminescence is monitored from evanescently excited, dye-doped polystyrene nanospheres (RS=20–80 nm) on a fused silica prism surface as a function of probe-sample geometry. The incident laser field is enhanced in the near-field of the probe tip, resulting in images with high sensitivity (σmin(approximate)2 Å2 in a 1 Hz detection bandwidth) and strongly subdiffraction-limited spatial resolution. At probe-sample distances greater than (approximate)λ/2, the images are dominated by far-field interference between (i) direct fluorescence from the molecular sample and (ii) indirect fluorescence from image dipoles induced in the atomic force microscope probe. Near-field "shadowing" of the molecular fluorescence by the probe also occurs and is studied as a function of probe-sample-detector geometry. Finally, effects of probe-sample proximity on the fluorescence emission spectrum are investigated. In summary, the data elucidate several novel near- and far-field molecular fluorescence enhancement effects relevant to further development of molecular and nanostructural spectroscopic methods with spatial resolution well below the diffraction limit. © 2001 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 8
    Electronic Resource
    Electronic Resource
    [s.l.] : Nature Publishing Group
    Nature 214 (1967), S. 671-674 
    ISSN: 1476-4687
    Source: Nature Archives 1869 - 2009
    Topics: Biology , Chemistry and Pharmacology , Medicine , Natural Sciences in General , Physics
    Notes: [Auszug] Chlortetracycline caused dramatic increases in intestinal weight of bacteria-laden and germ-free female mice only, the greatest in the former. Intestinal histamine and serotonin decreased in all mice except bacteria-laden females which showed increases in serotonin. Thus, sex and microbial status ...
    Type of Medium: Electronic Resource
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  • 9
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 110 (1999), S. 5149-5158 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Detailed investigations are described for the generation of open-shell radical complexes formed by unimolecular photolysis of closed-shell van der Waals precursors. As a specific test case, ultraviolet photolysis of slit-jet cooled Arn–H2S (n≤2) complexes at both 248 and 193 nm are shown to yield Ar–SH and Ar2–SH radical cluster species with surprisingly high efficiencies. Analysis of the laser induced fluorescence (LIF) spectra indicates that the radical complexes are produced with extensive van der Waals stretch/bend and overall rotational excitation, which is consistent with a simple ballistic model of the dissociation dynamics. The LIF spectra obtained as a function of expansion distance downstream provide clear evidence for remarkably efficient cooling of the newly formed radical cluster species by low-energy collisions with jet-cooled inert gas atoms at (approximate)10 K. Spectrally resolved Ar–SH and Ar2–SH LIF signals have been investigated as a function of Ar composition, which yields information on relative branching ratios for fragmentary (e.g., Ar2–H2S→Ar–SH+H+Ar) and nonfragmentary (e.g., Ar2–H2S→Ar2–SH+H) photolysis events. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 10
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 105 (1996), S. 11360-11363 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We describe a novel mechanism for efficient generation of open shell free-radical complexes via UV photolysis of the corresponding closed shell precursors. Ar–SH and Ar2–SH are detected following 248 nm excitation of Ar–H2S and Ar2–H2S. Of particular dynamical interest are the nonfragmentary channels in which no Ar atoms are ejected. © 1996 American Institute of Physics.
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