<p>Accurately modeling optical spectra with absolute radiometric intensities is vital for nuclear forensics applications that depend on characterizing optical emissions from energetic nuclear phenomena. This requires precise knowledge of the individual atomic transition probabilities, known as Einstein A-coefficients, for each emission line. Obtaining these values theoretically or experimentally is often impractical due to the complex electronic structures and the number of transitions involved in atoms relevant to nuclear applications. In this study, we explore the use of machine learning to predict the Einstein A coefficients for atomic transitions. Seven models were evaluated that ranged from deep learning to decision tree algorithms, and found that gradient boosting performed best, specifically the Extreme Gradient Boosting&#xa0;(XGB) architecture, achieving a precision of 86% across transitions of 36 elements. The model was cross-validated using published transition probabilities reported in the literature and applied to estimate Pu plasma temperatures from a previous experiment conducted at Savannah River National Laboratory.</p>