Reaction ergodography for silicon nitride bond formation in the laser-driven gas-phase reaction

Journal Article · Thu Jun 28 00:00:00 EDT 1990 · Journal of Physical Chemistry; (USA)

DOI:https://doi.org/10.1021/j100376a012· OSTI ID:6521032

Tachibana, Akitomo; Kurosaki, Yuzuru; Sera, Toshiaki; Tanaka, Eishi; Fueno, Hiroyuki; Yamabe, Tokio ^[1]

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1. Kyoto Univ. (Japan)

Reaction ergodography using IRC (intrinsic reaction coordinate) as a unique reaction path is studied for silicon nitride bond formation in the gas phase. This is a dehydrogenation reaction. Using a model system, we have obtained the activation energy 55.4 kcal/mol and the exothermic energy 2.8 kcal/mol (CISD+QC/6-31G{sup **}//HF/6-31G{sup *}). This is consistent with the experimentally observed activation energy 39 kcal/mol by Vasilyeva, Ginovker, Popov, and Repinsky (Izv. Sib. Otd. Akad. Nauk SSSR, Ser. Khim. Nauk 1979, 5, 54). The IRC reveals mode-specific vibrational excitation of SiH{sub 4} in the early stage of reaction, and additionally, that of NH{sub 3} just before the transition state, and successive strong charge-transfer interaction in the neighborhood of the transition state. The first finding is in agreement with the recent observations that 10.6 {mu}m (943.4 cm{sup {minus}1}) light emitted from CO{sub 2} laser is efficient for silicon nitride bond formation in the gas phase.

• OSTI ID: 6521032
• Journal Information: Journal of Physical Chemistry; (USA), Journal Name: Journal of Physical Chemistry; (USA) Vol. 94:13; ISSN 0022-3654; ISSN JPCHA
• Country of Publication: United States
• Language: English

Related Subjects

36 MATERIALS SCIENCE
360202* -- Ceramics
Cermets
& Refractories-- Structure & Phase Studies
BONDING
CALCULATION METHODS
CERAMICS
CHEMICAL REACTIONS
DEHYDROGENATION
FABRICATION
JOINING
MATHEMATICAL MODELS
MOLECULAR ORBITAL METHOD
NITRIDES
NITROGEN COMPOUNDS
PNICTIDES
SILICON COMPOUNDS
SILICON NITRIDES