Hannon J B, Kodambaka S, Ross F M, Tromp R M
IBM Research Division, T. J. Watson Research Center, Yorktown Heights, New York 10598, USA.
Nature. 2006 Mar 2;440(7080):69-71. doi: 10.1038/nature04574. Epub 2006 Jan 29.
Interest in nanowires continues to grow, fuelled in part by applications in nanotechnology. The ability to engineer nanowire properties makes them especially promising in nanoelectronics. Most silicon nanowires are grown using the vapour-liquid-solid (VLS) mechanism, in which the nanowire grows from a gold/silicon catalyst droplet during silicon chemical vapour deposition. Despite over 40 years of study, many aspects of VLS growth are not well understood. For example, in the conventional picture the catalyst droplet does not change during growth, and the nanowire sidewalls consist of clean silicon facets. Here we demonstrate that these assumptions are false for silicon nanowires grown on Si(111) under conditions where all of the experimental parameters (surface structure, gas cleanliness, and background contaminants) are carefully controlled. We show that gold diffusion during growth determines the length, shape, and sidewall properties of the nanowires. Gold from the catalyst droplets wets the nanowire sidewalls, eventually consuming the droplets and terminating VLS growth. Gold diffusion from the smaller droplets to the larger ones (Ostwald ripening) leads to nanowire diameters that change during growth. These results show that the silicon nanowire growth is fundamentally limited by gold diffusion: smooth, arbitrarily long nanowires cannot be grown without eliminating gold migration.
对纳米线的兴趣持续增长,部分原因是纳米技术中的应用推动。设计纳米线特性的能力使其在纳米电子学中特别有前景。大多数硅纳米线是通过气-液-固(VLS)机制生长的,在这种机制中,纳米线在硅化学气相沉积过程中从金/硅催化剂液滴生长出来。尽管经过了40多年的研究,但VLS生长的许多方面仍未得到很好的理解。例如,在传统观点中,催化剂液滴在生长过程中不会改变,并且纳米线的侧壁由干净的硅晶面组成。在这里,我们证明,在所有实验参数(表面结构、气体纯度和背景污染物)都得到仔细控制的条件下,对于在Si(111)上生长的硅纳米线,这些假设是错误的。我们表明,生长过程中的金扩散决定了纳米线的长度、形状和侧壁特性。来自催化剂液滴的金会浸润纳米线的侧壁,最终消耗掉液滴并终止VLS生长。金从小液滴向大液滴的扩散(奥斯特瓦尔德熟化)导致纳米线直径在生长过程中发生变化。这些结果表明,硅纳米线的生长从根本上受到金扩散的限制:如果不消除金的迁移,就无法生长出光滑、任意长的纳米线。