Density functional theory (DFT) method has been used to investigate geometries, electronic structures, and vibrational frequencies of alkali metal P 4 M 2 (M=Li, Na, and K) clusters and alkali earth metal P 4 M (M=Be, Mg, and Ca) clusters. Calculation results show that the square P42- dianion can coordinate with metal atoms to form the pyramidal P 4 M and the dipyramidal P 4 M 2 complexes maintaining the square P42- dianion structure. Molecular orbital (MO) analysis revealed that the square planar P42- dianion exhibits characteristic of π-aromaticity with six delocalized π electrons and maintains its structural and electronic integrity inside the P 4 M 2 and P 4 M clusters.