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Most elemental metals under ambient conditions adopt simple structures suchas BCC, FCC and HCP in specific groupings across the Periodic Table, and oncompression, many of these elements undergo transitions to surprisingly complexstructures, including open and low-symmetry phases not expected fromconventional free-electron based theories of metals. First-principlescalculations have been able to reproduce many observed structures andtransitions, but a unified, predictive theory of bonding that underlies thisbehavior is not yet in hand. We propose a remarkably simple theory based onlarge-scale high-throughput calculations of the elements over a broad range ofthermodynamic conditions. The results broaden the conventional concept ofmetallic bonding with a new perspective that both explains the stability ofdifferent simple structures as well as lower symmetry phases arising fromelectron localization at interstitial sites in these structures. The success ofthis simple framework reveals the important role of chemical interactions ingoverning the structures and electronic properties of simple metals.

Unified chemical theory of structure and bonding in elemental metals