Superconducting, plastic, and superionic states driven by four-membered lithium rings in a high-pressure lithium-lead compound

Abstract

Using a combination of crystal structure search methods, first-principles calculations, and machine learning potential based simulations, we explored the lithium-lead system and predicted five phases: I4/mcm LiPb2, Pnma LiPb, I4/mmm Li4Pb, C2/m Li5Pb, and Cmcm Li6Pb. Among them, I4/mmm Li4Pb displayed remarkable properties, including superconductivity, plasticity, and superionic behavior at varying temperature ranges. At lower temperatures, I4/mmm Li4Pb manifests superconductivity with a critical transition temperature of 4–5 K. Its superconducting behavior is attributed to the interplay between the B2 g vibration mode, which signifies the rotational motion of four-membered lithium rings within the stacking layer, and the participation of p-orbital electrons. As temperature rises, I4/mmm Li4Pb first transitions into a plastic phase, marked by continuous collective rotation of intralayer four-membered lithium rings, and then shows superionic behavior characterized by the emergence of interlayer lithium atom diffusion. These unique behaviors stem from stronger Li-Li bonds within four-membered lithium rings and a lower energy barrier for collective motion, distinct from interstitial localized electrons in electrides found in other lithium-based systems. This work provides an intriguing platform for exploring distinct states and establishes a correlation between various physical phenomena and the system's structure and bonding.

Source-reported materials — not catalogue approval

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