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  • American Institute of Physics (AIP)  (4)
  • 1
    Electronic Resource
    Electronic Resource
    The rotational spectrum and structure of chlorine peroxide (1989)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 91 (1989), S. 6588-6597 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The products of the ClO self-reaction have been studied in a flowing chemical reactor using submillimeter wave spectroscopy. The complete spectrum between 415 to 435 GHz has been measured as well as selected transitions in the range 285 to 415 GHz. The major products have been identified as the ClO dimer (Cl2O2) and chlorine dioxide (OClO). The observed rotational b-type spectra of the most abundant isotopic species35 ClOO35Cl and 37ClOO35Cl have been analyzed. The observed nuclear spin statistics for the main species, the relative abundance of the lesser species, and the structure determination demonstrate unambigiously that the ClO dimer must possess identical chlorine atoms in a peroxide structure. The rotational constants as well as a complete set of quartic centrifugal distortion constants have been determined. Structural parameters for the vibronic ground state have been calculated: rOO=142.59(21) pm, rClO=170.44(4) pm, (angle)ClOO=110.07(1)° and dihedral angle=81.03(1)°. Rotational transitions in the first excited torsional state have been measured and analyzed for the isotopic species 35,35 and 35,37. An effective molecular structure for the first torsional excited state has been calculated. A torsional frequency has been derived from relative intensity measurements and the cis and the trans barrier heights estimated.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.457377
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  • 2
    Electronic Resource
    Electronic Resource
    Measurement of the V–T energy transfer rates of highly excited 2A1 NO2 (1994)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 100 (1994), S. 8040-8046 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Production of electronic ground state NO2 (2A1) from 248 nm photolysis of HNO3 was detected by laser induced fluorescence (LIF). A growth in the LIF signal was observed following the photolysis and has been interpreted as the relaxation of NO2 through the higher vibrational levels of the X(2A1) state; an energy region where the probe laser photodissociates the NO2 instead of inducing fluorescence. The rate coefficients for NO2 relaxation through these high vibrational levels were determined by fits of time resolved LIF signal to a stepladder kinetic model. The results of the kinetic analysis suggest that the observed relaxation begins at the 2B2 threshold near 9500 cm−1 and extends downward through approximately 5 vibrational levels of the ground electronic surface. The derived quenching rate coefficients (in units of 10−12 cm3 molecule−1 s−1) are 0.51±0.05, 1.0±0.1, 1.4±0.2, 2.6±0.6, and 8.7±1.1 for Ar, He, N2, O2, and CO2 collision partners, respectively. The discrepancies between these coefficients and previous literature values are rationalized in terms of a dependence of the vibrational relaxation rate on total internal energy.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.466797
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  • 3
    Electronic Resource
    Electronic Resource
    The OBrO C(2A2)←X(2B1) absorption spectrum (1997)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 107 (1997), S. 2300-2307 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The highly structured visible absorption spectrum of the bromine dioxide radical, OBrO, has been observed in the 15 500–26 000 cm−1 region. The spectrum is dominated by a long progression in the Br–O symmetric stretching motion (ν1′) and a series of short progressions built on the bending mode (ν2′); there are no features associated with the excitation of the antisymmetric stretching mode (ν3′). The spectrum also contains numerous transitions originating from the (0,1,0) and (1,0,0) vibrational levels of the electronic ground state, X(2B1). A simultaneous fit to all of the observed vibronic features yielded the frequencies ν1″=799.4 cm−1, ν2″=317.5 cm−1, ω1′=641.5 cm−1, ω2′=210.7 cm−1, and a band origin T0=15 863 cm−1. Franck–Condon simulations combined with ab initio calculations of the four lowest OBrO doublet electronic states identify the spectrum as arising from the C(2A2)←X(2B1) electronic transition. © 1997 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.474606
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  • 4
    Electronic Resource
    Electronic Resource
    Pressure dependence and metastable state formation in the photolysis of dichlorine monoxide (Cl2O) (1996)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 104 (1996), S. 2857-2868 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The photodissociation of dichlorine monoxide (Cl2O) was studied using broadband flash photolysis to investigate the influence of variations in the photolysis wavelength domain, bath gas pressure and bath gas identity on the yield and temporal dependence of the ClO product. ClO yields were independent of bath gas pressure when the photolysis spectral band extended to 200 nm (quartz cutoff) but for photolysis restricted to wavelengths longer than about 250 nm, ClO yields decreased with increasing bath gas pressure and there was a pressure-dependent delay in the formation of ClO. Under these conditions, a weak, highly structured absorption spectrum was observed in the range 16 600–26 000 cm−1 with a lifetime on the order of 500 ms. A portion of the spectrum could be analyzed (22 000–26 000 cm−1) which showed progressions having differences of 283, 443, and 505 cm−1. Ab initio calculations were performed to evaluate vertical excitation energies and oscillator strengths from the lowest-energy singlet (X 1A1) or triplet (1 3B1) states to various excited states. The calculations indicated that the 2 3A2←1 3B1 transition has an unusually large oscillator strength. The transition energy, 3.05 eV, is consistent with the observed metastable spectrum. The observed pressure dependence of ClO formation could be modeled using a mechanism which assumed that Cl2O excitation at wavelengths longer than about 300 nm leads to rapid intersystem crossing to two metastable states in the triplet manifold. These states undergo competitive dissociation to ClO+Cl and collisional relaxation to the ground state. The dynamics of Cl2O may serve as a model for other molecules of importance in the earth's lower stratosphere such as ClONO2 where filtering of the solar spectrum by ozone restricts photolysis to the weak tail of the absorption continuum. © 1996 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.471109
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