Creating 3D Nanoparticle Structural Space via Data Augmentation to Bidirectionally Predict Nanoparticle Mixture's Purity, Size, and Shape from Extinction Spectra

Abstract Nanoparticle (NP) characterization is essential because diverse shapes, sizes, and morphologies inevitably occur in as‐synthesized NP mixtures, profoundly impacting their properties and applications. Currently, the only technique to concurrently determine these structural parameters is electron microscopy, but it is time‐intensive and tedious. Here, we create a three‐dimensional (3D) NP structural space to concurrently determine the purity, size, and shape of 1000 sets of as‐synthesized Ag nanocubes mixtures containing interfering nanospheres and nanowires from their extinction spectra, attaining low predictive errors at 2.7–7.9 %. We first use plasmonically‐driven feature enrichment to extract localized surface plasmon resonance attributes from spectra and establish a lasso regressor (LR) model to predict purity, size, and shape. Leveraging the learned LR, we artificially generate 425,592 augmented extinction spectra to overcome data scarcity and create a comprehensive NP structural space to bidirectionally predict extinction spectra from structural parameters with <4 % error. Our interpretable NP structural space further elucidates the two higher‐order combined electric dipole, quadrupole, and magnetic dipole as the critical structural parameter predictors. By incorporating other NP shapes and mixtures′ extinction spectra, we anticipate our approach, especially the data augmentation, can create a fully generalizable NP structural space to drive on‐demand, autonomous synthesis‐characterization platforms.