Molecular sp3-like Reactivity of Metastable Au4Si near Its Deep Eutectic Point Enables Low-Temperature SiC Formation
Jhong-Ren Huang1, Yi-Hsin Liu2, Satoshi Kameoka3
1Department of Mechanic Engineering, National Taiwan University of Science and Technology, No. 43, Sec. 4, Keelung Rd., Da'an Dist., Taipei City 106335, Taiwan.
Abstract:
Metastable states near deep eutectic points are typically regarded as transient intermediates preceding phase separation, yet their potential chemical reactivity remains largely unexplored. Here, we demonstrate that metastable Au-Si bonding configurations derived from Au4Si near its deep eutectic temperature exhibit molecule-like reactivity associated with an sp3-like local bonding environment, enabling direct Si-C bond formation at temperatures as low as 636 K. Using a high-vacuum coevaporation platform, Au-Si species generated during coevaporation react with carbon clusters to produce SiC accompanied by Au segregation, whereas elemental Si under identical conditions remains chemically inert. Raman spectroscopy and X-ray photoelectron spectroscopy reveal that SiC formation occurs only within a narrow temperature window centered at the eutectic point and displays nonmonotonic temperature dependence inconsistent with conventional catalytic or vapor-liquid-solid mechanisms. These results provide experimental evidence that eutectic metastable bonding configurations can transiently adopt molecule-like characteristics, thereby enabling unconventional low-temperature reaction pathways in metal-semiconductor systems.
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