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We introduce a fully automated machine-learning framework for reconstructing physically consistent SOC-resolved PECs across independent electronic-structure calculations with different basis-set representations. The approach combines generative data augmentation using a conditional Wasserstein Generative Adversarial Network with gradient penalty (cWGAN-GP) with supervised regression models (Ridge Regression, Gradient Boosting, and Extremely Randomized Trees) to learn the relationship between raw SOC-affected PECs, spin\u2013orbit composition tables, and their physically corrected counterparts. Using MgCa as a demonstration system, SOC-resolved PECs and spectroscopic constants were computed at the MRCI level for the ground and 26 low-lying excited states. Models trained on a single manually corrected reference basis accurately predict physically corrected PEC energies for independent basis sets, achieving sub-percent deviations in dissociation energies while preserving asymptotic limits, equilibrium geometries, and fine-structure splittings without explicit constraints. This framework eliminates manual postprocessing of SOC-mixed PECs and provides a scalable strategy for consistent spin\u2013orbit treatment in high-level electronic-structure workflows.<\/jats:p>","DOI":"10.1021\/acs.jctc.6c01257","type":"journal-article","created":{"date-parts":[[2026,9,16]],"date-time":"2026-09-16T17:02:04Z","timestamp":1789578124000},"page":"10366-10380","source":"Crossref","is-referenced-by-count":0,"title":["Machine Learning\nMeets Spin\u2013Orbit Coupling:\nReconstruction of Spin\u2013Orbit-Mixed Potential Energy Curves\nin MgCa"],"prefix":"10.1021","volume":"22","author":[{"given":"Giovanna C.","family":"Rizkallah","sequence":"first","affiliation":[{"name":"Universita\u0308t Rostock , , ,","place":["Rostock, Germany, 18059"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4788-3288","authenticated-orcid":true,"given":"Samir N.","family":"Tohme","sequence":"additional","affiliation":[{"name":"Universita\u0308t Hamburg , , ,","place":["Hamburg, Germany, 22761"]},{"name":"Lehigh Carbon Community College , , ,","place":["Schnecksville, Pennsylvania, United States, 18078"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,16]]},"reference":[{"key":"2026101310074225200_cit1","volume-title":"Molecular Spectra and\nMolecular Structure","author":"Huber","year":"2013"},{"issue":"2","key":"2026101310074225200_cit2","doi-asserted-by":"publisher","first-page":"287","DOI":"10.1006\/jmsp.2001.8345","article-title":"DiRef, a Database of References Associated with the\nSpectra of Diatomic Molecules","volume":"207","author":"Bernath","year":"2001","journal-title":"J. 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