Yoo Soohaeng, Zhao Jijun, Wang Jinlan, Zeng Xiao Cheng
Department of Chemistry and Center for Materials Research & Analysis, University of Nebraska, Lincoln, Nebraska 68588, USA.
J Am Chem Soc. 2004 Oct 27;126(42):13845-9. doi: 10.1021/ja046861f.
We have performed an unbiased search for the lowest-energy geometric structures of medium-sized silicon clusters SiN (27 < or = N < or = 39) using a genetic algorithm and nonorthogonal-tight-binding method, followed by a refining and biased search using basin-hopping method coupled with density-functional theory. We show that the carbon fullerene cages are most likely generic cage motifs ("magic cages") to form low-lying stuffed-cage silicon clusters (beyond the size N > 27). An empirical rule that provides optimal "stuffing/cage" combinations for constructing low-energy endohedral silicon fullerenes is suggested, with a hope that it can provide guidance to future synthesis of "bucky" silicon.
我们使用遗传算法和非正交紧束缚方法,对中等尺寸硅团簇SiN(27≤N≤39)的最低能量几何结构进行了无偏搜索,随后使用盆地跳跃方法结合密度泛函理论进行了优化和有偏搜索。我们表明,碳富勒烯笼极有可能是形成低能填充笼硅团簇(尺寸超过N>27)的通用笼型图案(“魔法笼”)。提出了一条经验规则,用于为构建低能内嵌硅富勒烯提供最佳的“填充/笼”组合,希望能为未来“巴基”硅的合成提供指导。