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The structures of compressed rubidium polyhydrides, RbH  n   with  n >1, and their evolution under pressure are studied using density functional theory calculations. These phases, which start to stabilize at only  P =2 GPa, consist of Rb +  cations and one or more of the following species: H −  anions, H 2  molecules, and  ${{\rm H}{{- \hfill \atop 3\hfill}}}$  molecules. The latter motif, the simplest example of a three‐center four‐electron bond, is found in the most stable structures, RbH 5  and RbH 3 , which metallize above 200 GPa. At the highest pressures studied, our evolutionary searches find an RbH 6  phase which contains polymeric ( ${{\rm H}{{- \hfill \atop 3\hfill}}}$ ) ∞  chains that show signs of one‐dimensional liquid‐like behavior.

Rubidium Polyhydrides Under Pressure: Emergence of the Linear H 3 − Species