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First Lidar Observations of Mesospheric Hydroxyl
For the first time, ground-based lidars have been used to identify and detect ground-state (V
Certain properties of the hydroxyl emission
Intensity and rotational temperature variations of oxygen hydrogen bands in airglow
Temporal variations in night-time hydroxyl rotational temperature.
Airborne and groundbased OH measurements showing short-term temporal variations in OH rotational temperature are presented. These variations are interpreted in terms of a dynamic model of the OH emitting layer in which the intensity variations result from the changes in temperature the OH layer undergoes as it moves during the night.
Rates of interaction of vibrationally excited hydroxyl /v = 9/ with diatomic and small polyatomic molecules.
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Infrared maser emission from interstellar hydroxyl molecules
The energy structure and transition rates of the OH radical were studied in rotational and vibrational energies to provide the basis for studies of the population distributions under various exciting mechanisms. The absorption of ultra-violet or near infrared radiation which might explain the microwave emission was examined, as well as the absorption of low temperature blackbody radiation and collisions with molecular hydrogen. The results of the population studies were applied to the transfer equation, and a model of a uniform spherical cloud of OH was used with the pumping process which occurs uniformly throughout the region. The emission is unsaturated and the intensity is an exponential function of the size of the cloud for high pumping rates, and the region of unsaturated emission shrinks for lower pumping rates until the entire region is saturated, the intensity then becoming a linear function of the size of the emitting cloud.
Determination of atomic oxygen density from rocket borne measurement of hydroxyl airglow
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Very long baseline interferometric observations of the hydroxyl masers in VY Canis Majoris
Results are presented for spectral-line VLBI observations of the OH emission from VY CMa. The main-line (1665 and 1667 MHz) emission was mapped with an angular resolution of 0.02 arcsec by analyzing interferometer phase data. The main-line emission comes from many maser components of apparent size less than 0.03 arcsec which are separated by up to 0.5 arcsec. New maser features near the center of the OH spectra were detected and found to lie within the region encompassed by the low-velocity OH emission. The 1612-MHz emission was mapped by Fourier inversion of the VLBI data from two baselines. All spatially isolated maser components appeared smaller than 0.15 arcsec; however, the maser emission is very complex at most velocities. Maser components within a velocity range of 1.3 km/s are often separated by more than 1 arcsec, while components more than 10 km/s apart in each emission complex are often coincident to 0.2 arcsec.
Rate constant for the reaction of hydroxyl radical with formaldehyde over the temperature range 228-362 K
Absolute rate constants for the reaction OH ? H2CO measured over the temperature range 228-362 K using the flash photolysis-resonance fluorescence technique are given. The results are independent of variations in H2CO concentration, total pressure Ar concentration, and flash intensity (i.e., initial OH concentration). The rate constant is found to be invariant with temperature in this range, the best representation being k sub 1 = (1.05 ? or - 0.11) x 10 to the 11th power cu cm molecule(-1) s(-1) where the error is two standard deviations. This result is compared with previous absolute and relative determinations of k sub 1. The reaction is also discussed from a theoretical point of view.
Rate constant for the reaction of hydroxyl radical with formaldehyde over the temperature range 228-362 K
Absolute rate constants for the reaction OH + H2CO have been measured over the temperature range 228-362 K using the flash photolysis-resonance fluorescence technique. The results were independent of variations in forbidden H2CO, total pressure of forbidden Ar and flash intensity (i.e., initial forbidden OH). The rate constant was found to be invariant with temperature in this range, the best representation being k1 = (1.05 + or - 0.11) x 10 to the -11th cu cm/molecule sec where the error is two standard deviations. This result is compared with previous absolute and relative determinations of k1. The reaction is also discussed from a theoretical point of view.
Stratospheric hydroxyl radical concentrations - New limitations suggested by observations of gaseous and particulate sulfur
A one-dimensional aerosol model is employed in investigating the sensitivity of the stratospheric distributions of gaseous sulfur compounds and sulfate aerosol particles to changes in OH and CS2 concentrations, in eddy diffusion coefficients, and in important chemical rate constants. By comparing model predictions with recent observational data for SO2, OCS, and particulates, it is found that, with regard to atmospheric sulfur, CS2 is only a secondary source of sulfur for the stratosphere relative to OCS and that background tropospheric CS2 concentrations by volume are likely to be less than 70 parts per trillion. It is also established that under stratospheric conditions the rate coefficients for the reactions of OH with OCS and CS2 may be substantially smaller than the room temperature laboratory values of Kurylo (1978).
Kinetics of the gas-phase reaction between hydroxyl and carbonyl sulfide over the temperature range 300-517 K
By use of a discharge-flow resonance-fluorescence method the rate constant for the title reaction has been measured at five temperatures in the range 300-520 K. The Arrhenius expression is k(OH + OCS) = (1.3 + or - 0.3) x 10 to the -12th exp/-(2300 + or - 100)/T/ cu cm/s. Mass spectrometry has been used to detect the product HS and to collect some information about its reactivity. This study has carefully avoided the pitfalls associated with possible photolysis of reactants and complications due to H2S impurity in carbonyl sulfide that may have marred previous studies. This study has confirmed that the rate constant for this reaction is so much lower than the value originally used in computer modeling of the upper and lower atmosphere that conclusions about the relative importance of photolysis of OCS and of the reaction OH + OCS in the stratosphere must now be reassessed. The reaction OH + OCS has little significance for atmospheric chemistry.
Rate constants for the gas-phase reaction between hydroxyl and hydrogen sulfide over the temperature range 228-518 K
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Comments on laser-excited fluorescence of the hydroxyl radical: Relaxation coefficients at atmospheric pressure, appendix 5
The lifetime of the excited state of a atom or molecule is often determined from the rate of fluorescence decay originating as a function of buffer gas pressure, an accurate determination is made of the rates of collision induced transitions away from the excited state. Deconvolution can in principle be employed to resolve fluorescence times shorter than the response times of the system. However, attainable reproducibility and accuracy in actual experiments usually set a limit beyond which no meaningful results are expected. Prudence thus dictates that the results of deconvolution be viewed with extreme caution whenever fluorescence time much shorter than the response of times of the system are indicated.
Fundamental Equations of the LIF Hydroxyl Measurements, Appendix a
The equation relating OH concentration to the observed detector count rate for a given laser flux is defined. That equation, which will be referred to henceforth as the central equation for absolute sensitivity, will be cast in terms of standard spectroscopic quantities such as oscillator strengths, Hoenl-London factors, rotational and vibrational quantum numbers, etc., such that it may be tested directly under laboratory conditions. The working expressions used by each of the OH laser induced fluorescence (LIF) groups will be related to this central equation, thereby establishing a common language for the comparison of experimental results and the definition of LIF system performance. The relevant structural details of the OH radical via a spectroscopic description of the energy levels and transitions employed in the LIF method are detailed. The central equation relating observed count rate to absolute concentration will be derived, and that equation will be related to the observed quantities cited by each of the experimental groups engaged in the measurement of OH in the Earth's atmosphere.
Mechanism of the atmospheric oxidation of sulfur dioxide - Catalysis by hydroxyl radicals
A flash photolysis/resonance fluorescence technique was used to investigate the decay of OH due to the reaction OH + SO2 (+M) to HOSO2 (+M). In the presence of small amounts of NO (10 to the 14th per cu cm), the decays deviated from the normal semilogarithmic linearity due to reformation of OH. On the basis of computer simulations of the decay curves, it is suggested that the reactions HOSO2 + O2 to HO2 + SO3 (k3), and HO2 + HO to OH + NO2 are the likely subsequent steps in SO2 oxidation. The upper limit for the binding energy of HOSO2 relative to OH + SO2 is estimated to be 32 kcal/mol. The atmospheric implications of a catalytic oxidation mechanism are briefly discussed.
Operational overview of Wallops Island instrument intercomparison - Carbon monoxide, nitric oxide, and hydroxyl instrumentation
NASA has initiated the Global Tropospheric Experiment (GTE) for the study of the chemistry of the global troposphere. One phase of GTE, Chemical Instrumentation Test and Evaluation (CITE), is concerned with the development and validation of measurement techniques for trace species which play important roles in the tropospheric chemical cycles. In connection with CITE 1 an intercomparison of instruments is conducted for the measurement of CO, NO, and OH. These species have been identified as critical for an understanding of homogeneous gas-phase chemistry in the troposphere. The present paper provides an operational overview of the first of three instrument intercomparison field missions conducted as part of GTE/CITE 1. The missions include one ground-based and two airborne missions, and were designed to characterize current capability of measuring ambient levels of CO, NO, and OH.
Measurements of superequilibrium hydroxyl concentrations in turbulent nonpremixed flames using saturated fluorescence
The first quantitative, time- and space-resolved measurements have been obtained for probability density functions of OH concentration in nonpremixed flames. Measurements using single-pulse, laser-saturated fluorescence in laminar, transitional, and turbulent nonpremixed H2-air flames provide unambiguous evidence for substantial OH superequilibrium concentrations, in qualitative agreement with predictions of laminar and turbulent combustion models. The average degree of superequilibrium, OH/OH(AE), is typically 4-5 near the jet exit and approaches unity far downstream. The maximum instantaneous OH concentration measured in transitional and turbulent H2-air flames is about 6 x 10 to the 16th molecules/cc, in accord with the maximum determined by partial equilibrium thermodynamic calculations and with the maximum OH concentrations measured in premixed H2-air flames.