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Disorder-Driven Ionic Mobility Edge and Localization-Driven Dendrite Formation in Solid Electrolytes
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DOI：10.1002/aenm.71274.png)
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Abstract
En 中文
Dendrite formation in solid electrolytes remains a central obstacle to reliable solid-state batteries, yet its microscopic origin is debated. A unified framework is presented in which dendrites emerge from disorder-driven localization of ionic transport. A disorder parameter σE, defined by the variance of migration energy barriers, controls the topology of the percolation backbone above the ionic mobility edge Ec. While Ec is set by the mean barrier and remains invariant under σE, increasing disorder depletes active conducting pathways, driving a transition from extended conduction to localized transport. This connectivity transition produces filamentary current channels under applied bias; the resulting flux focusing and electric-field amplification at filament tips provide a direct mechanism for dendrite nucleation. Subsequent growth follows transport-limited diffusion-limited aggregation dynamics, yielding fractal morphologies with Df ≈ 1.7. The critical current density follows jcrit = j0 exp(−σE, eff/kBT), linking microscopic energy-landscape statistics to macroscopic electrochemical stability. The resulting disorder–current phase diagram reveals a nonequilibrium transition between stable and dendritic regimes. These results establish transport localization as a fundamental transport-mediated mechanism of dendrite formation, indicating that narrowing the distribution of migration barriers, reducing the mean barrier alone, is key to stable solid electrolytes.
Keywords:
chemical physics
condensed matter physics
ionic bonding
materials science
nucleation
percolation
percolation threshold
phase diagram
protein filament
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