Bimetallic clusters have aroused increased attention because of the ability to tune their own properties by changing size, shape, and doping. In present work, a structural search of the global minimum for divalent bimetal Be₂Mg_n (n = 1–20) clusters are performed by utilizing CALYPSO structural searching method with subsequent DFT optimization. We investigate the evolution of geometries, electronic properties, and nature of bonding from small to medium-sized clusters. It is found that the structural transition from hollow 3D structures to filled cage-like frameworks emerges at n = 10 for Be₂Mg_n clusters, which is obviously earlier than that of Mg_n clusters. The Be atoms prefer the surface sites in small cluster size, then one Be atom tend to embed itself inside the magnesium motif. At the number of Mg larger than eighteen, two Be atoms have been completely encapsulated by caged magnesium frameworks. In all Be₂Mg_n clusters, the partial charge transfer from Mg to Be takes place. An increase in the occupations of the Be-2p and Mg-3p orbitals reveals the increasing metallic behavior of Be₂Mg_n clusters. The analysis of stability shows that the cluster stability can be enhanced by Be atoms doping and the Be₂Mg₈ cluster possesses robust stability across the cluster size range of n = 1–20. There is s-p hybridization between the Be and Mg atoms leading to stronger Be-Mg bonds in Be₂Mg₈ cluster. This finding is supported by the multi-center bonds and Mayer bond order analysis.

双金属簇由于能够通过改变尺寸，形状和掺杂来调整其自身特性而引起了越来越多的关注。在目前的工作中， 通过使用CALYPSO结构搜索方法以及随后的DFT优化，对二价双金属Be ₂ Mg _n（n = 1-20）簇的全局最小值进行结构搜索。我们研究了几何形状，电子特性以及从中小型簇到结合层的性质的演变。据发现，从空心3D结构填充所述结构转变笼状的框架，在出现Ñ  = 10成为₂的Mg _Ñ簇，这显然是早于Mg的_Ñ集群。Be原子更喜欢簇形较小的表面位，然后一个Be原子倾向于将自身嵌入镁基序内。Mg大于18时，两个Be原子已被笼状镁骨架完全包封。在所有的Be ₂ Mg _n簇中，发生了从Mg到Be的部分电荷转移。Be- 2p和Mg- 3p轨道的占据增加表明Be ₂ Mg _n团簇的金属行为增加。稳定性分析表明，可以通过掺杂Be原子来增强簇的稳定性，并且Be ₂ Mg ₈簇在整个簇尺寸范围内都具有较强的稳定性。n  = 1-20。Be和Mg原子之间存在s - p杂化，从而在Be ₂ Mg ₈簇中形成更强的Be-Mg键。多中心债券和Mayer债券定单分析支持了这一发现。