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Abstract Machine learning (ML) is relied on for materials spectroscopy. It is challenging to make ML models fail because statistical correlations can mimic the physics without causality. Here, using a benchmark band‐excitation piezoresponse force microscopy polarization spectroscopy (BEPS) dataset the pitfalls of the so‐called “better”, “faster”, and “less‐biased” ML of electromechanical switching are demonstrated and overcome. Using a toy and real experimental dataset, it is demonstrated how linear nontemporal ML methods result in physically reasonable embedding (eigenvalues) while producing nonsensical eigenvectors and generated spectra, promoting misleading interpretations. A new method of unsupervised multimodal hyperspectral analysis of BEPS is demonstrated using long‐short‐term memory (LSTM) β‐variational autoencoders (β‐VAEs) . By including LSTM neurons, the ordinal nature of ferroelectric switching is considered. To improve the interpretability of the latent space, a variational Kullback–Leibler‐divergency regularization is imposed . Finally, regularization scheduling of β as a disentanglement metric is leveraged to reduce user bias. Combining these experiment‐inspired modifications enables the automated detection of ferroelectric switching mechanisms, including a complex two‐step, three‐state one. Ultimately, this work provides a robust ML method for the rapid discovery of electromechanical switching mechanisms in ferroelectrics and is applicable to other multimodal hyperspectral materials spectroscopies.more » « less
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