Kinetic studies of atmospherically relevant silicon chemistry Part I: Silicon atom reactions

文献情報

出版日 2008-11-21

DOI 10.1039/B812946K

インパクトファクター 3.676

著者

Juan C. Gómez Martín, Mark A. Blitz, John M. C. Plane

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要旨

Atomic silicon is generated by meteoric ablation in the Earth’s upper atmosphere (70–110 km). The reactions of Si(3PJ) atoms with several atmospherically relevant species were studied by the pulsed laser photolysis of a Si atom precursor (typically PheSiH3), followed by time-resolved laser induced fluorescence at 251.43 nm (Si(3p23P0→ 4s 3P1)). This yielded: k(Si + O2, 190–500 K) = 9.49 × 10−11 + 1.80 × 10−10× exp(−T/115 K) cm3 molecule−1 s−1 (uncertainty ≤±15%), in good accord with recent high-level theoretical calculations but in marked disagreement with previous experimental work; k(Si + O3, 190–293 K) = (4.0 ± 0.5) × 10−10 cm3 molecule−1 s−1; k(Si + CO2, 293 K) ≤ 1.2 × 10−14 cm3 molecule−1 s−1; and k(Si + H2O, 293 K) ≤ 2.6 × 10−13 cm3 molecule−1 s−1. These results are explained using a combination of quantum chemistry calculations and long-range capture theory. The quenching rate coefficients k(Si(1D2) + N2, 293 K) = (4.0 ± 0.7) × 10−11 cm3 molecule−1 s−1 and k(Si(1D2) + H2O, 293 K) = (2.3 ± 0.3) × 10−10 cm3 molecule−1 s−1 were also determined.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

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