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An unexpected superconductivity enhancement is reported in decompressed In2Se3. The onset of superconductivity in In2Se3 occurs at 41.3 GPa with a critical temperature (Tc) of 3.7 K, peaking at 47.1 GPa. The striking observation shows that this layered chalcogenide remains superconducting in decompression down to 10.7 GPa. More surprisingly, the highest Tc that occurs at lower decompression pressures is 8.2 K, a twofold increase in the same crystal structure as in compression. It is found that the evolution of Tc is driven by the pressure‐induced R‐3m to I‐43d structural transition and significant softening of phonons and gentle variation of carrier concentration combined in the pressure quench. The novel decompression‐induced superconductivity enhancement implies that it is possible to maintain pressure‐induced superconductivity at lower or even ambient pressures with better superconducting performance.
Superconductivity enhancement in pressure quenching is observed in the layered material In2Se3. In situ high‐pressure resistance and magnetic measurements reveal a twofold increase of Tc at lower decompression pressure. It is found that the superconductivity enhancement in decompressed In2Se3 is driven by the significant softening of phonons and gentle variation of carrier concentration combined in the pressure quench.