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NASA NTRS1997

Kinetics of the Reactions of F((sup 2)P) and Cl((sup 2)P) with HNO3

The kinetics of the reactions of HNO3 with fluorine (k(sub 1)) and Chlorine (k(sub 2)) atoms have been studied by using a time-resolved long-path laser absorption technique to monitor the appearance of product NO3 radicals following 351-nm pulsed laser photolysis of X2/HNO3/He mixtures (X = F,Cl). Absolute rate coefficients for the F((sup 2)P) + HNO reaction have been determined over the temperature range 260-373 K. Between 260 and 320 K, the data are adequately represented by the Arrhenius expression k(sub 1)(T) = (6.0 +/- 2.6) x 10(exp -12) exp[(40 +/- 120)/T]cu cm/(molecule.s). Between 335 and 373 K, the rate coefficient is found to be (2.0 +/- 0.3) x 10(exp -11)cu cm/(molecule.s) independent of temperature. The observed temperature dependence suggests that reaction proceeds via competing direct abstraction and complex pathways. No NO3 production was observed in the experiments with X equals Cl, thus establishing that k(sub 2)(298 K) is less than 2 x 10(exp -16) cu cm/(molecule.s). The Cl((sup 2)P) + HNO reaction was also investigated by using a pulsed laser photolysis-resonance fluorescence technique to monitor the decay of Cl((sup 2)P). Upper limit values for k(sub 2) obtained from these experiments, in units of 10(exp -16)cu cm/(molecule.s), are 13 at 298 K and 10 at 400 K.

Wine, P. H.↗

NASA NTRS1997

Optical and Atomic Force Microscopy Characterization of PbI2 Quantum Dots

Lead iodide (PbI2) clusters were synthesized from the chemical reaction of NaI (or KI) with Pb(NO3)2 in H2O, D2O, CH3OH, and C3H7OH media. The observation of the absorption features above 350 nm with the help of integrating sphere accessory strongly suggests the quantum dot formation of PbI2 in solution. Spectral comparison between the synthesized PbI2 clusters in solution and PbI2 nanophase by impregnation of PbI2 in four different pore-sized porous silica indicates that the PbI2 cluster size in solution is less than 2.5 nm in lateral dimension. Atomic force microscopy (AFM) measurements show that the PbL clusters deposited onto three different molecularly flat surfaces are single-layered. The measured height is 1.0 - 0.1 nm. The swollen layer thickness can be attributed to the intralayer contraction from the strong lateral interaction among PbI2 molecules, which is supported by ab initio calculation. Raman scattering measurement of LO and TO modes of PbI2 in bulk and in the confined state were also conducted in 50-150 cu cm region. The observed three bands at 74, %, 106 1/cm are assigned to TO2, LO2, and LO, mode, respectively. The relatively small red-shift in LO modes may be caused by the surface phonon polaritons of PbI2 nanophase in the porous silica.

Mu, R.↗