O2 Oxidation and Sublimation Kinetics of Single Silicon Nanoparticles at 1200–2050 K: Variation of Reaction Rates, Evolution of Structural and Optical Properties, and the Active-to-Passive Transition

Rodriguez, Daniel J.; Lau, Chris Y.; Friese, Abigail M.; Long, Bryan A.; Anderson, Scott L.

doi:10.1021/acs.jpcc.2c05985

Title: O₂ Oxidation and Sublimation Kinetics of Single Silicon Nanoparticles at 1200–2050 K: Variation of Reaction Rates, Evolution of Structural and Optical Properties, and the Active-to-Passive Transition

Journal Article · Tue Nov 01 00:00:00 UTC 2022 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.2c05985 · OSTI ID:1900403

^[1]; Lau, Chris Y. ^[2]; Friese, Abigail M. ^[2]; Long, Bryan A. ^[2];

^[2]

Univ. of Utah, Salt Lake City, UT (United States); University of Utah
Univ. of Utah, Salt Lake City, UT (United States)

Sublimation and O₂ etching kinetics for a series of individual silicon (Si) nanoparticles (NPs) were studied for NP temperatures (T_NP) from 1200 to 2050 K, using a single NP mass spectrometry technique. Sublimation was significant for T_NP > 1700 K, with rates reasonably well fit to Arrhenius kinetics, but evolving, particularly during initial heating. O₂ etching efficiencies varied from NP-to-NP and with changing T_NP, but also evolved dramatically over time. For T_NP ≤ 1500 K, NPs were observed to passivate after losing 30 to 50% of the initial NP mass. At higher T_NP, etching efficiency decreased over time, but never passivated. Interestingly, bulk Si passivation has not been observed for the range of T_NP and O₂ pressures used here, and a model was developed to test the effects of several NP-specific mechanistic parameters on both the initial and time-dependent etching behavior. As a result, the optical properties of the hot NPs were also found to evolve as the NPs etched, particularly during the initial fast mass loss, and correlations between emission intensities and etching kinetics were examined.

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Research Organization:: Univ. of Utah, Salt Lake City, UT (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0018049

OSTI ID:: 1900403

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 44 Vol. 126; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: O2 Oxidation and Sublimation Kinetics of Single Silicon Nanoparticles at 1200–2050 K: Variation of Reaction Rates, Evolution of Structural and Optical Properties, and the Active-to-Passive Transition

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Title: O₂ Oxidation and Sublimation Kinetics of Single Silicon Nanoparticles at 1200–2050 K: Variation of Reaction Rates, Evolution of Structural and Optical Properties, and the Active-to-Passive Transition