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Photoinduced Structural Instability Toward the Superionic Phase Transition in Cu2S
Gaël Privault1, Kaito En-Ya2, Keito Sano3
1Institute of Pure and Applied Sciences, University of Tsukuba, Tsukuba 305-8573, Japan.
Abstract:
Copper(I) sulfide (Cu2S) undergoes a semiconductor-to-superionic phase transition associated with the destabilization of the ordered Cu sublattice. Herein, we investigated the structural dynamics of photoexcited Cu2S using time-resolved electron diffraction from picoseconds to milliseconds. The measurements reveal a rapid suppression (80%-90%) of semiconducting phase superlattice reflections in ∼10 ps, indicating prompt destabilization of Cu ordering. This process is accompanied by a slower lattice expansion of approximately 100 ps, observed as a shift of Bragg diffraction peaks corresponding to a lattice strain of ∼0.7%. The suppression of the superlattice reflections exhibits a fluence threshold, indicating a critical excitation density for destabilizing the ordered Cu sublattice. Density functional theory calculations show that photoexcitation populates antibonding states, weakening Cu-S bonds, and driving the observed structural destabilization. These findings reveal the ultrafast microscopic pathway toward the superionic phase in Cu2S and provide insights into photoinduced structural dynamics in superionic materials.
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