Theory of Linear Optical Absorption in B_12 Clusters: Role of the geometry

Physics – Atomic and Molecular Clusters

Scientific paper

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12 pages, 5 tables, and 10 figures (included); submitted for publication

Scientific paper

Boron clusters have been widely studied theoretically for their geometrical properties and electronic structure using a variety of methodologies. An important cluster of boron is the B$_{12}$ cluster whose two main isomers have distinct geometries, namely, icosahedral ($I_{h}$) and quasi planar ($C_{3v}$). In this paper we investigate the linear optical absorption spectrum of these two B$_{12}$ structures with the aim of examining the role of geometry on the optical properties of clusters. The optical absorption calculations are performed using both the semi-empirical and the ab initio approaches. The semi-empirical approach uses a wave function methodology employing the INDO model Hamiltonian, coupled with large-scale configuration interaction (CI) calculations, to account for the electron-correlation effects. The \emph{ab initio} calculations are performed within a time-dependent-density-functional-theory (TDDFT) methodology. The results for the two approaches are in very good qualitative agreement with each other. Quantitatively speaking, results agree with each other in the lower energy region, while in the higher energy region, features predicted by the TDDFT approach are red-shifted as compared to the INDO-CI results. Both the approaches predict that the optical absorption begins at much lower energies in the icosahedral cluster as compared to the planar one, a fact which can be utilized in experiments to distinguish between the two geometries. At higher energies, both the isomers exhibit plasmon-like excitations. 73,1 4%

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