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Tracking Ultrafast Ion Diffusion Dynamics in AgCrSe2 Superionic Conductor

Jianmin Yang1,2, Lin Xie1,3,*, Mingyuan Hu1, Yingpeng Qi4, Jun Li5, Baohai Jia1, Jianghe Feng1, Zijing Chen4, Michel Bosman2 et al.

Dao Xiang4,6,† and Jiaqing He1,7,‡

  • *Contact author: xielin@gbu.edu.cn
  • †Contact author: dxiang@sjtu.edu.cn
  • ‡Contact author: hejq@sustech.edu.cn
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Phys. Rev. X 16, 021024 – Published 1 May, 2026

DOI: https://doi.org/10.1103/s6rh-7219

Abstract

Superionic conductors (SICs) exhibit liquidlike ionic diffusivities while maintaining a periodic crystalline lattice, making them promising candidates for applications in fuel cells, solid-state electrolytes, and thermoelectric materials. The transient local structures of mobile ions and their cooperative interactions with the host lattice are of pivotal importance regarding both the ion and heat conduction in SICs. However, accurately capturing the structural evolution of mobile ions remains a significant challenge due to the inherent complexities involved. Here, we employed ultrafast electron diffraction (UED) with femtosecond-temporal and angstrom-spatial resolution to resolve the structural evolution of mobile Ag+ ions in AgCrSe2. Our experiments identify a critical process originating from localized Ag+ vibrations at the long-range-ordered lattice sites to a formation of short-range-correlated Ag+ trimer structures through a drastic contraction of the Ag+─Ag+ bond from approximately 3.68 to approximately 3.00 Å in 1.97 ps. Combining real-time time-dependent density-functional-theory and molecular dynamics simulation, we further reveal the crucial role of these contracted trimer structures in enabling fast Ag+ diffusion by opening up excess free volume and reducing local energy barriers. Such an intimate relation between fast diffusion and local lattice variations is not exclusive and can be extended beyond AgCrSe2 to materials such as Li10XP2S12 (X=Si, Ge, Sn). The ability to track ion diffusion with UED also provides new avenues for exploring the atomistic mechanisms of fast ion diffusion in next-generation solid-state electrolytes, fuel cells, and ion transport membranes.

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Popular Summary

Superionic conductors are unusual materials that are structurally solid yet allow ions to move almost as freely as in liquids, offering great promise for safer and more efficient energy technologies. However, the atomic processes responsible for this extraordinary mobility have remained elusive. Using ultrafast electron diffraction with femtosecond temporal resolution and atomic spatial resolution, we captured the motion of Ag+ ions in the superionic conductor AgCrSe2 in real time. We find that the mobile ions do not migrate independently, but briefly assemble into small clusters with profoundly shortened Ag+─Ag+ bonds. This transient clustering creates additional free volume in the lattice and lowers the energy barriers for ion transport. These findings provide direct atomic-scale insight into liquidlike ion transport in a solid and suggest strategies for designing high-performance solid-state energy materials.

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Phys. Rev. X 16, 021024– Published 1 May, 2026
  • Received 7 November 2025
  • Accepted 24 March 2026
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