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Ionic transport in silver iodide (AgI) is not a simple Poisson process. Molecular dynamics simulations reveal time-correlated ion hopping, indicating a many-body diffusion mechanism in AgI polymorphs.

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Area of Science:

  • Solid-state ionics
  • Materials science
  • Computational physics

Background:

  • Ionic transport in solids is often modeled as independent diffusion events (hops).
  • This assumption implies diffusion follows a Poisson process, leading to Arrhenius expressions for transport coefficients.

Purpose of the Study:

  • To investigate the validity of the independent hopping assumption in AgI polymorphs.
  • To compare ion hopping rates with Poisson distributions using molecular dynamics simulations.

Main Methods:

  • Molecular dynamics simulations were performed on low-temperature B1, B3, and B4 AgI polymorphs.
  • Rates of ion hopping were analyzed and compared against Poisson distributions.

Main Results:

  • Diffusion in all AgI polymorphs studied was found to be a non-Poisson process.
  • Ion hopping events were strongly correlated in time.
  • In B1 AgI, diffusion coefficients approximated Arrhenius behavior, but with altered physical parameter significance.
  • In low-temperature B3 and B4 AgI, diffusion involved concerted motion of multiple ions in closed loops.

Conclusions:

  • The assumption of independent ion hopping is not valid for AgI polymorphs.
  • Diffusion in AgI is a many-body process, particularly in B3 and B4 phases characterized by loop-like ionic motion.
  • Standard Arrhenius expressions may not accurately reflect the underlying physics of diffusion in these materials.