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The preparation of compounds with novel atomic oxidation states and emergent properties is of fundamental interest in chemistry. As s-block elements, alkali-earth metals invariably show a +2 formal oxidation state at normal conditions, and among them, barium (Ba) presents the strongest chemical reactivity. Herein, we propose that novel valence states of Ba can be achieved in pressure-induced chalcogenides, where it also shows a feature of 5d-elements. First-principles swarm-intelligence structural search calculations identify three nove
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