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Two‐component relativistic time‐dependent density functional theory calculations with spin‐orbit coupling predict yellow and orange–red absorption for BiPh 5  and BiMe 5 , respectively, providing an excellent explanation for their respective violet and blue–violet colors. According to the calculations, the visible absorption is clearly attributable to a single transition from a ligand‐based HOMO to a low‐energy LUMO with a significant contribution from a relativistically stabilized Bi 6s orbital. Surprisingly, scalar releativistic calculations completely fail to reproduce the observed visible absorption and place it at the violet/near‐UV borderline instead.

The Blue–Violet Color of Pentamethylbismuth: A Visible Spin‐Orbit Effect