ABSTRACT:We have studied the structure and geometry of neutral and charged atomic clusters consisting of Ga and As atoms via ab initio Hartree-Fock (HF) and second-order Møller-Plesset methods. The Ga m As n cluster with m = n composition prefers a nontetrahedral geometry in the charge neutral (q = 0) state. These clusters tend to be stable in tetrahedral geometry when appropriately charged. The Ga m As n cluster with m = n composition (1:1 ratio of Ga to As atoms) tends to be stable in a tetrahedral geometry in the charge neutral (q = 0) state. With increasing size of the cluster, the geometry of Ga n As n cluster approaches the zinc-belende-type crystalline structure.