The MSI binary maps generated through PCA were then aligned with the linearly unmixed LCO data (Figure -o, Suppl. Fig. and). Here, the heterogeneity in the hyperspectral imaging data, that contained highly aggregated, q-FTAA dominant features (purple), and less aggregated forms of Aβ fibrils that were h-FTAA dominant (green) (Figure -l) were used as guidance for class-assignment of subsequent orthogonal projection to latent structures discriminant analysis (OPLS-DA). MSI pixel data within the generated ROI and that were corresponding between both imaging modalities were selected for subsequent statistical data analysis.