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

Literature Information

Publication Date 2008-11-21
DOI 10.1039/B812946K
Impact Factor 3.676
Authors

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


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Abstract

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.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
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Self-citation Rate: 10.3%
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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