Structures of Small Tantalum Cluster Anions: Experiment and Theory

• Published in: The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory Vol. 125; no. 15; pp. 3135 - 3145
• Main Authors: Kraft, Manuel, Flores, Jesús R, Klopper, Wim, Kappes, Manfred M, Schooss, Detlef
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 22-04-2021
• Subjects: A: Structure, Spectroscopy, and Reactivity of Molecules and Clusters
• ISSN: 1089-5639; 1520-5215
• DOI: 10.1021/acs.jpca.1c01250

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 Ta6 – and Ta8 – as well as structures based on the pentagonal bipyramid (Ta7 – and Ta9 –). Ta10 ––Ta12 – are defective icosahedral structures and Ta13 – 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.