Gate-pulse-induced recombination, known as the charge pumping (CP), is a fundamental carrier recombination process, and has been utilized as a method for analyzing electrical properties of defects (or dangling bonds) at the transistor interfaces, which is now recognized to be well-matured and conventional. Nevertheless, neither the origin (the bonding configuration) of the defects responsible for the CP, nor their detailed recombination sequence has been clarified yet for Si metal-oxide-semiconductor (MOS) interfaces. In order to address these problems, we investigated the CP under spin resonance conditions at temperatures ranging from 27 to 300 K in Si(100) n-type MOS transistors. We obtained evidence that Pb0 and E' centers, the two major dangling bonds at (and near) the Si(100) interface, participate in the CP recombination process. We also show that the spin-dependent CP process is explained by the formation of electron-electron spin pairs, which in turn reveals that the CP via Pb0 and E' centers is inherently a two-electron process.