perhaps due to poor alignment of low-frequency phonon eigenmodes with ion migration pathways in some materials. A new metric that incorporates both frequencies and alignments-the mean alignment-weighted frequency-is more strongly correlated with migration barriers (R 2 = 0.25). Materials in this study with the lowest migration barriers consistently exhibit the lowest mean alignment-weighted frequencies, suggesting the utility of this metric for filtering out materials with high barriers in screening efforts. Comparisons to previous studies suggest that phonon band centers may be correlated with migration barriers only in compositionally similar materials, and that adding alignment information may enable more reliable predictions among more diverse sets of materials. These results quantify the promise of using phonon frequencies and alignments, perhaps in combination with other properties, to efficiently screen for materials with high multivalent ionic conductivity.