Zuo Jingning, Zhang Lili, Chen Bole, He Kaihua, Dai Wei, Ding Kewei, Lu Cheng
School of Mathematics and Physics, China University of Geosciences (Wuhan), Wuhan 430074, People's Republic of China.
School of Science, Chongqing University of Posts and Telecommunications, Chongqing 400065, People's Republic of China.
J Phys Condens Matter. 2023 Sep 28;36(1). doi: 10.1088/1361-648X/acfc0c.
Doping metal heteroatoms is an effective strategy to regulate the geometric and electronic structure of boron based nanoclusters. However, the exploration of the ground state structures of metal-boron-based nanoclusters is still a challenge duo to the complexity of the bonding interactions between heterogeneous atoms and boron cluster and the number of isomers on the potential energy surface increases exponentially with cluster size. Here, we use the CALYPSO cluster structural search method in combination with density functional theory calculations to study the geometries and electronic properties of anionic boron clusters doped with plutonium (PuBn-,= 10-20). Our results show that the medium-sized PuB14-cluster exhibits excellent stability with highest occupied molecular orbital-lowest unoccupied molecular orbital energy gap of 2.30 eV. The remarkable stability of the anionic PuB14-cluster is due to the robust interactions between the Pu metal and the Bskeleton, along with the strong covalent interactions between the B atoms. These findings enrich the geometric structure database of metal doped clusters and provide valuable insights for the future synthesis of boron based nanomaterials.
掺杂金属杂原子是调控硼基纳米团簇几何结构和电子结构的有效策略。然而，由于异质原子与硼团簇之间键合相互作用的复杂性以及势能面上异构体的数量随团簇尺寸呈指数增加，探索金属硼基纳米团簇的基态结构仍然是一项挑战。在此，我们使用CALYPSO团簇结构搜索方法结合密度泛函理论计算，研究掺杂钚的阴离子硼团簇（PuBn -，n = 10 - 20）的几何结构和电子性质。我们的结果表明，中等尺寸的PuB14 -团簇表现出优异的稳定性，最高占据分子轨道 - 最低未占据分子轨道能隙为2.30 eV。阴离子PuB14 -团簇的显著稳定性归因于Pu金属与B骨架之间的强相互作用以及B原子之间的强共价相互作用。这些发现丰富了金属掺杂团簇的几何结构数据库，并为未来硼基纳米材料的合成提供了有价值的见解。
