The role of specific atomic-scale defects involved in total ionizing dose radiation in the metal–oxide–semiconductor field-effect transistors of the 1980s and 1990s was identified in large part with electron paramagnetic resonance (EPR) techniques. The techniques involved in those studies were classical EPR and, to a lesser extent, electrically detected magnetic resonance (EDMR). We show that somewhat more sophisticated resonance-based measurements can be fruitfully applied to explore the atomic-scale basic mechanisms of the significantly more complex, generally messier, and much smaller devices of the present day. We present multifield and frequency EDMR measurements in which the response is observed via spin-dependent leakage currents, spin-dependent charge pumping, and spin-dependent gated diode recombination currents. We also exploit isotopic substitution, replacing hydrogen with deuterium, monitoring the isotopic effects on the resonance response. The approaches utilized in this paper should be applicable to radiation damage studies in a wide variety of emerging materials and devices.