Chem. Sci., 2026, Accepted Manuscript DOI: 10.1039/D6SC04497B, Edge Article Erica Sutcliffe, Jonathan P Aalto, Ryan G Hadt Paramagnetic molecules are promising quantum sensors with dimensions and environmental compatibility inaccessible to solid-state defects. Realizing this promise, however, requires optical methods for initializing and reading out coherent spin dynamics....