Large-scale first-principles configuration-interaction calculations of optical absorption in boron clusters

Abstract

We have performed systematic large-scale all-electron correlated calculations on boron clusters Bn(n = 2 - 5), to study their linear optical absorption spectra. Several possible isomers of each cluster were considered, and their geometries were optimized at the coupled-cluster singles doubles (CCSD) level of theory. Using the optimized ground-state geometries, the excited states of different clusters were computed using the multi-reference singles-doubles configuration–interaction (MRSDCI) approach, which includes electron correlation effects at a sophisticated level. These CI wave functions were used to compute the transition dipole matrix elements connecting the ground and various excited states of different clusters, eventually leading to their linear absorption spectra. The convergence of our results with respect to the basis sets, and the size of the CI expansion were carefully examined. The contribution of configurations to many body wave-function of various excited states suggests that the excitations involved are collective, plasmonic type.

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C/C++⁵ chemistry⁸ computer science⁸ fortran⁷ GPU¹ physics¹¹ programming³ python⁶ simulation²

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