a detailed understanding of the dynamics of photogenerated charge carriers has remained incomplete due to the complexity of the microscopic landscape of amorphous systems. The band structure formalism that leads to accurate descriptions of well-ordered crystalline semiconductors fails to adequately describe the behavior of amorphous systems, which are characterized by an exponentially decaying density of states in energies that extend into the classically forbidden band gap (see Figure 1a). Due to this large density of native defects and mid-gap states such as dangling bonds (DBs, see Figure 1a), the dynamics of photogenerated carriers in a-Si:H resemble to those of organic semiconductors, where the charge transport may also occur by hopping between nearby localized states having similar carrier mobility values. Also radiative recombination occurs between localized, strongly exchange-coupled electron-hole (e-h) polaron pairs. In addition, the photogenerated carriers are similarly localized in both systems. For these reasons, there might be valuable insight to be gained by applying some of the models of spin-dependent recombination processes developed in the field of organic semiconductors [10][11][12] to the a-Si:H system, as done here.It is an experimentally challenging task to probe photocarriers in an energy-resolved manner so that the effects of wavefunction localization in such amorphous systems might be elucidated. Magnetic resonance experiments can be devised so that only a desired subset of the total photogenerated carrier population is probed. [13] For example, electrically detected magnetic resonance [14] is sensitive only to those carriers which participate in conduction, so that the g-factors and hyperfine coupling strengths of electrons or holes near their respective mobility edges may be revealed. Optically detected magnetic resonance [15][16][17] and light-induced electron spin resonance [18] are sensitive to localized spin ½ electrons or holes that are trapped in deep defect states and do not participate in transport. Powerful as these techniques are for probing the local environment of photogenerated charge carriers, it is desirable to supplement them by a careful investigation of the steady-state photoluminescence (PL) and photocurrent (PC) efficiency, so that practical a-Si:H devices operating in the steady-state regime may benefit from the thorough understanding of microscopic carriers dynamics.Herein, the magneto-photoluminescence (MPL) of localized photocarriers and magneto-photoconductivity (MPC) of delocalized photocarriers in amorphous hydrogenated silicon (a-Si:H) films and devices, respectively, are investigated. Both responses are caused by mixing of spin sublevels in the photogenerated electron-hole (e-h) pairs that alters their recombination and dissociation rates. The spin mixing occurs by a combination of hyperfine interaction (HFI) between spin ½ photocarriers and neighboring 29 Si and 1 H nuclei, and the Δg mechanism which originates from a difference in the Landé g-factors of el...