Structures of Small Tantalum Cluster Anions: Experiment and Theory

Abstract

We present a study of the structural evolution of tantalum cluster anions Ta n − , 6 ≤ n ≤ 13 using a combination of trapped ion electron diffraction (TIED) experiments with a variety of electronic structure methods. A genetic algorithm has been employed to establish a set of likely structures for each cluster, their geometries and energetics have been studied by density functional theory (DFT), random phase approximation, and two-component (2C) DFT methods, which include spin−orbit coupling. We find octahedral structures for Ta 6 − and Ta 8 − as well as structures based on the pentagonal bipyramid (Ta 7 − and Ta 9 − ). Ta 10 − −Ta 12 − are defective icosahedral structures and Ta 13 − is a distorted icosahedron. For most clusters, we find a good agreement between the theoretically predicted ground-state structures, especially those determined by the 2C method and the TIED results.

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