Chem. Sci., 2026, Accepted Manuscript DOI: 10.1039/D6SC01160H, Edge Article Helen Saejung Clifford, Aniruddha Seal, Laura Gagliardi Accurate simulation of excited-state bond-rearrangement dynamics remains a major challenge since photoinduced reactions can often involve significant changes in electronic structure along excited-state reaction pathways. Describing such processes requires an...