Dynamic Behavior, Optical Response, and Reactivity of Li–Na Nanoalloy Clusters: A Combined CDFT and ITA Perspective

are investigated by exploring their potential energy surfaces using density functional theory (DFT) calculations coupled with the ABCluster global optimization program. Structural and electronic properties of the bimetallic (Li, Na) clusters are explored through quantum chemical calculations. The optimized geometries reveal that in bimetallic Li-Na clusters, mostly Li atoms tend to be encapsulated within the sodium framework, while Na atoms preferentially occupy peripheral positions. For a given cluster size, the relative stability of different Li-Na compositions have been examined to identify the structurally most favorable configurations. To the best of our knowledge, for the first time, we have investigated the dynamic behavior and optical properties of bimetallic Li-Na clusters. Atom-centered density matrix propagation simulation reveals that the Li-Na bonding interactions are dynamic, indicating the kinetic stability of the binary cluster. The nonlinear optical responses show that the polarizability and hyperpolarizability can be tuned by size and Li:Na composition. Furthermore, a comprehensive conceptual DFT study combined with information theoretic approach of (Li, Na) clusters reported here, has not been previously explored. The outcomes guide designing atomically precise, thermally stable, and composition-tunable nanoalloys for researchers.