Lithium-Projected Phonon Spectral Distributions as Robust Descriptors of Ionic Conductivity in Solid Electrolytes

Abstract

Lattice dynamics are widely invoked in the design of solid electrolytes, yet phonon information is commonly compressed into a band center or another scalar softness measure. Here we test whether the complete lithium-projected phonon density of states (Li-PDOS) provides a reproducible descriptor of experimental room-temperature ionic conductivity. MatterSim forces and Phonopy were used to generate harmonic total and Li-projected spectra for crystallographically resolved entries in the OBELiX dataset. A composition and structure audit defined a primary cohort of 260 materials (212 train and 48 test), a strict cohort of 241, and an exact-composition cohort of 168. Across 20 independently generated phonon-calculation database comparisons, the mean Wasserstein-1 distance was 0.542 THz for total DOS and 0.731 THz for Li-PDOS, revealing broad agreement but systematic, projection-dependent softening. Higher conductivity was associated with redistribution of normalized Li spectral weight toward low frequencies: in the untouched test set, the Li fractions below 2 and 5 THz had Spearman coefficients of 0.333 and 0.374, while the 5$\%$ cumulative-frequency quantile had a coefficient of $-0.393$. A Wasserstein kernel on the full Li-PDOS achieved held-out $R^2=0.444$, compared with 0.012 for total DOS and 0.181 for a static composition--structure kernel. The Li model remained stable in the strict ($R^2=0.462$) and exact ($R^2=0.451$) cohorts. Family adjustment attenuated scalar associations, and Li-versus-total whole-spectrum dependence was cohort sensitive. The results therefore support mobile-ion-resolved spectral distributions as useful comparative screening descriptors, not as a universal causal softness law.