Kinetics of SiHCl3 and SiCl4 evolution in Si(s)-HCl(g) system simulated by ab-initio MO

Nagahiro Saito, Takahiro Ishizaki, Akio Fuwa

    Research output: Contribution to journalArticle

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    Abstract

    A reaction model for a HCl(g)-Si(s) system is proposed in this study as follows: first, SiCl2(g) and H2(g) are produced by a heterogeneous surface reaction, and then SiHCl3(g) and SiH2Cl2(g) are produced by the homogeneous reaction between SiCl2(g) and HCl(g) and between SiCl2(g) and H2(g), respectively; finally, SiCl4(g) and SiHCl3(g) are produced by the homogeneous reaction between SiHCl3(g) and HCl(g) and between SiH2Cl2(g) and HCl(g), respectively. The mechanism in the first heterogeneous surface reaction step has been studied extensively in the past. However, the detail of the subsequent homogeneous reactions has not yet been understood. It is important to get information of the chemical kinetics of the reactions derived from the reaction intermediate of SiCl2(g) in the SiCl2(g)-HCl(g)-H2(g) system, so the most plausible elementary reactions of reversible unimolecular fission and chain reaction are proposed here. The structures of the molecules formed in these reactions are optimized using the minimization principle of energy calculated by ab-initio molecular orbital method and also their rate constants are calculated by conventional transition state theory. Using these rate constants, the ordinary differential equations are solved on mass balance, and the time dependent concentration profile of respective chemical species and the prior reaction paths are discussed in this study.

    Original languageEnglish
    Pages (from-to)383-392
    Number of pages10
    Journalmaterials transactions, jim
    Volume41
    Issue number3
    Publication statusPublished - 2000 Mar

    Fingerprint

    Surface reactions
    Rate constants
    Reaction intermediates
    Kinetics
    kinetics
    Molecular orbitals
    Ordinary differential equations
    Reaction kinetics
    Molecules
    surface reactions
    dichlorosilane
    reaction intermediates
    mass balance
    fission
    molecular orbitals
    reaction kinetics
    differential equations
    optimization
    profiles

    ASJC Scopus subject areas

    • Engineering(all)

    Cite this

    Kinetics of SiHCl3 and SiCl4 evolution in Si(s)-HCl(g) system simulated by ab-initio MO. / Saito, Nagahiro; Ishizaki, Takahiro; Fuwa, Akio.

    In: materials transactions, jim, Vol. 41, No. 3, 03.2000, p. 383-392.

    Research output: Contribution to journalArticle

    Saito, Nagahiro ; Ishizaki, Takahiro ; Fuwa, Akio. / Kinetics of SiHCl3 and SiCl4 evolution in Si(s)-HCl(g) system simulated by ab-initio MO. In: materials transactions, jim. 2000 ; Vol. 41, No. 3. pp. 383-392.
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