Detailed kinetic modeling of silicon nanoparticle formation chemistry via automated mechanism generation

Hsi Wu Wong, Xuegeng Li, Mark T. Swihart, Linda J. Broadbelt*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

38 Scopus citations

Abstract

Thermal decomposition of silane can be used to produce silicon nanoparticles, which have attracted great interest in recent years because of their novel optical and electronic properties. However, these silicon nanoparticles are also an important source of paniculate contamination leading to yield loss in conventional semiconductor processing. In both cases, a fundamental knowledge of the reaction kinetics of particle formation is needed to understand and control the nucleation of silicon particles. In this work, detailed kinetic modeling of silicon nanoparticle formation chemistry was carried out using automated reaction mechanism generation. Literature values, linear free-energy relationships (LFERs), and a group additivity approach were incorporated to specify the rate parameters and thermochemical properties of the species in the system. New criteria for terminating the mechanisms generated were also developed and compared, and their suitability for handling an unbounded system was evaluated. Four different reaction conditions were analyzed, and the models predicted that the critical particle sizes were Si 5 for an initial H 2/SiH 4 molar ratio of 90:10 at 1023 K and Si 4 for the same initial composition at 1200 K. For an initial H 2/SiH 4 molar ratio of 99:1, the critical particle size was larger than or equal to Si 7 for both temperatures, but it was not possible to determine the exact critical particle size because of limitations in computational resources. Finally, the reaction pathways leading to the formation of nanoparticles up to the critical size were analyzed, and the important species in the pathways were elucidated.

Original languageEnglish (US)
Pages (from-to)10122-10132
Number of pages11
JournalJournal of Physical Chemistry A
Volume108
Issue number46
DOIs
StatePublished - Nov 18 2004

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

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