Anion Photoelectron Spectroscopy and Quantum Chemistry Calculations of Gas-Phase TaSi̅ and TaSi̅ Clusters: Structural Determination, Bonding Characteristics, and Multiplicity of Structural Forms.

This study explores the structures and chemical bonding properties of TaSi̅ and TaSi̅ clusters by employing anion photoelectron spectroscopy and theoretical computations. Utilizing CALYPSO and ABCluster programs for initial structure prediction, B3LYP hybrid functional for optimization, and CCSD(T)/def2-TZVPPD level for energy calculations, the research identifies the most stable isomers of these clusters. Key findings include the identification of two coexisting low-energy isomers for TaSi̅, exhibiting Ta-endohedral fullerene-like cage structures, and the lowest-energy structures of TaSi̅ and TaSi̅ anions can be considered as derived from the TaSi̅ superatom cluster. The study enhances the understanding of group 14 element chemistry and guides the design of novel inorganic metallic compounds, potentially impacting materials science.