Abstract

Neutral, anionic, and cationic B₃Al^0/−/+_n (n = 2–6) clusters were systematically explored using density functional theory and coupled cluster CCSD(T) methods to investigate the structural evolution of small mixed aluminum–boron clusters. The lowest energy structures of these clusters were obtained using an unbiased global minimum search, and their structural growth behaviors are discussed. The three boron atoms in B₃Al^0/−/+_n preferentially form a stable triangle, with additional Al atoms occupying the periphery of the boron triangle. For small clusters of n ≤ 3, the studied clusters show planar two–dimensional configurations. When n ≥ 4, the clusters prefer three–dimensional configurations. Average binding energies, fragmentation energies, second–order differences, HOMO–LUMO gaps, ionization potentials and electron affinities are discussed in detail. For cationic B₃Al⁺_n (n = 2–6) clusters, the even n systems are more stable than the odd n systems, while the stabilities of neutral B₃Al_n and anionic B₃Al⁻_n clusters do not change significantly with growing n. The infrared spectrum and photoelectron spectroscopy of these clusters are simulated, which will be useful for future experimental research. We also compare the chemical bonding of neutral B₃Al_n (n = 2–6) clusters with their ionic clusters by AdNDP analysis.

Graphic Abstract

中文翻译：

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硼铝混合团簇B 3 Al n0 /-/ +的原子结构，稳定性，电子性质和化学键合（n = 2–6）

摘要

利用密度泛函理论和耦合簇CCSD（T）方法系统研究了中性，阴离子和阳离子B ₃ Al ^{0 /-/ +} _n （n = 2–6）簇，以研究小型铝硼混合簇的结构演化。这些团簇的最低能量结构是使用无偏全局最小搜索获得的，并讨论了它们的结构生长行为。B ₃ Al ^{0 /-/ +} _n中的三个硼原子 优先形成一个稳定的三角形，其余的Al原子占据了硼三角形的外围。对于n≤3的小簇，研究的簇显示出平面二维构型。当n≥4时，群集更喜欢三维配置。详细讨论了平均结合能，碎片能，二阶差，HOMO-LUMO间隙，电离势和电子亲和力。对于阳离子B ₃ Al ⁺ _n （n = 2–6）团簇，偶数n系统比奇数n系统更稳定，而中性B ₃ Al _n和阴离子B ₃ Al ^- _n的稳定性 随着n的增长，聚类变化不大。对这些团簇的红外光谱和光电子能谱进行了模拟，将为以后的实验研究提供参考。我们还通过AdNDP分析比较了中性B ₃ Al _n（n = 2–6）簇与离子簇的化学键合。

图形摘要