Solid-State Dealloying Enables Local Symmetry Breaking in Ternary Intermetallic Thin Films

Metastable quantum materials often occupy narrow composition windows with local symmetries distinct from competing equilibrium structures. These features open pathways for realizing qualitatively new electronic properties within a similar chemical subspace while at the same time complicating their deterministic synthesis. Here we illustrate a post-growth solid-state dealloying process using epitaxial ternary thin films in the La–Ag–Ge chemical space to realize a diffraction-averaged centrosymmetric superconducting structure. The process converts polar $P{6}_{3}mc$-LaAgGe into diffraction-averaged centrosymmetric AlB${}_2$-type $P6\mathrm{/}mmm$ La-Ag-Ge through net Ag loss during annealing at 800–900 ${}^{\circ }$C. Atomic-resolution electron microscopy reveals local Ag–Ge displacements of both signs relative to the planar configuration, consistent with local inversion-symmetry-breaking distortions. The converted films exhibit composition-dependent superconductivity with critical temperatures below 1 K and in-plane upper critical fields that exceed the weak-coupling Pauli-field estimate by a factor of approximately 6 in the thinnest superconducting films. These results establish epitaxial solid-state dealloying as a route to phase-selective synthesis of metastable phases, offering control over atomic-scale structural configurations and their interplay with emergent electronic properties.