Theory and Computation methods for the Design and Reaction of Nonomolecules

(1)开发了高效的理论和计算方法以及并行化算法，可用于可靠水平的高速从头算和密度泛函计算。(2)通过引入非常大的甲硅烷基基团，从理论上预测了稳定的硅-硅三键化合物，这是目前主族化学中广泛关注的焦点。(3)系统地研究了熵效应的温度依赖性，以预测代表性金属富勒烯的异构体分布，例如Ca@C_<72>、Ca@C_<74>、Ca@C_<82>和La@C_<82>。(4)La_2@C_<80>中两个La原子的随机圆周运动可以通过附着外面给电子分子（例如二硅丙烷）来高度控制。预计受限运动将有助于感应独特的电子或磁场。 N@C60 和 P@C60 中 N 和 P 的自旋密度也通过外面添加二硅丙烷来控制。还验证了内嵌有机分子掺杂如何改变单壁碳纳米管的电子性质。(5)研究了金属掺杂的硅和锗团簇的结构和电子性质，揭示了内嵌结构的形成如何依赖于团簇的尺寸。还研究了硅和锗多面体分子的同芳香性的调制和调节。

(1)Efficient theoretical and computational methods as well as parallelization algorithms were developed, which are useful for high-speed ab initio and density functional calculations at reliable levels.(2)By introducing very bulky silyl groups, stable silicon-silicon triply bonded compounds were theoretically predicted which are currently the focus of considerable interest in main group chemistry.(3)Temperature dependence of entropy effects were systematically investigated to predict the isomer distributions of representative metallofullerenes such as Ca@C_<72>, Ca@C_<74>, Ca@C_<82>, and La@C_<82>.(4)The random circular motion of two La atoms in La_2@C_<80> can be highly controlled by attaching exohedrally electron-donating molecules such as disilirane. It is expected that the restricted motion will help to induce a unique electronic or magnetic field. The spin densities on N and P in N@C60 and P@C60 are also controlled upon exohedral addition of disilirane. It is also verified how the electronic properties of single-walled carbon nanotubes are modified by endohedral organomolecule-doping.(5)Structural and electronic properties of metal-doped silicon and germanium clusters were investigated to reveal how the formation of endohedral structures depend on the size of clusters. Modulation and tuning of homoaromaticity of silicon and germanium polyhedral molecules are also investigated.