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用于纳米结构半导体和电介质合成的类醚硅锗氢化物。

Ether-like Si-Ge hydrides for applications in synthesis of nanostructured semiconductors and dielectrics.

作者信息

Tice Jesse B, Weng Change, Tolle John, D'Costa Vijay R, Singh Rachna, Menendez Jose, Kouvetakis John, Chizmeshya Andrew V G

机构信息

Department of Chemistry and Biochemistry, Arizona State University, Tempe, AZ 85287-1604, USA.

出版信息

Dalton Trans. 2009 Sep 14(34):6773-82. doi: 10.1039/b908280h. Epub 2009 Jul 15.

DOI:10.1039/b908280h
PMID:19690688
Abstract

Hydrolysis reactions of silyl-germyl triflates are used to produce ether-like Si-Ge hydride compounds including H(3)SiOSiH(3) and the previously unknown O(SiH(2)GeH(3))(2). The structural, energetic and vibrational properties of the latter were investigated by experimental and quantum chemical simulation methods. A combined Raman, infrared and theoretical analysis indicated that the compound consists of an equal mixture of linear and gauche isomers in analogy to the butane-like H(3)GeSiH(2)SiH(2)GeH(3) with an exceedingly small torsional barrier of approximately 0.2 kcal mol(-1). This is also corroborated by thermochemistry simulations which indicate that the energy difference between the isomers is less than 1 kcal mol(-1). Proof-of-principle depositions of O(SiH(2)GeH(3))(2) at 500 degrees C on Si(100) yielded nearly stoichiometric Si(2)Ge(2)O materials, closely reflecting the composition of the molecular core. A complete characterization of the film by RBS, XTEM, Raman and IR ellipsometry revealed the presence of Si(0.30)Ge(0.70) quantum dots embedded within an amorphous matrix of Si-Ge-O suboxide, as required for the fabrication of high performance nonvolatile memory devices. The use of readily available starting materials coupled with facile purification and high yields also makes the above molecular approach an attractive synthesis route to H(3)SiOSiH(3) with industrial applications in the formation of Si-O-N high-k gate materials in high-mobility SiGe based transistors.

摘要

甲硅烷基锗基三氟甲磺酸酯的水解反应被用于制备醚类硅 - 锗氢化物化合物,包括H(3)SiOSiH(3)和此前未知的O(SiH(2)GeH(3))(2)。通过实验和量子化学模拟方法研究了后者的结构、能量和振动性质。拉曼光谱、红外光谱和理论分析相结合表明,该化合物由线性异构体和gauche异构体的等量混合物组成,类似于丁烷类的H(3)GeSiH(2)SiH(2)GeH(3),其扭转势垒极小,约为0.2 kcal mol(-1)。热化学模拟也证实了这一点,模拟结果表明异构体之间的能量差小于1 kcal mol(-1)。在500℃下将O(SiH(2)GeH(3))(2)原理性沉积在Si(100)上,得到了近乎化学计量比的Si(2)Ge(2)O材料,紧密反映了分子核心的组成。通过卢瑟福背散射谱(RBS)、高分辨透射电子显微镜(XTEM)、拉曼光谱和红外椭偏光谱对薄膜进行的全面表征揭示,在制造高性能非易失性存储器件所需的Si-Ge-O低价氧化物非晶基质中存在Si(0.30)Ge(0.70)量子点。使用容易获得的起始原料,再加上简便的纯化方法和高收率,也使得上述分子方法成为合成H(3)SiOSiH(3)的一种有吸引力的合成路线,在基于高迁移率SiGe的晶体管中形成Si-O-N高k栅极材料方面具有工业应用价值。

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