Abstract
<jats:title>Abstract</jats:title> <jats:p>Diluted magnetic semiconductors (DMSs) based on ZnO doped with transition metals have attracted significant attention due to their potential application in spintronic devices. However, the realization of intrinsic ferromagnetism in such systems remains controversial, primarily due to difficulties in achieving stable p-type conductivity. In this study, Zn 0.95 Mn 0.05 O thin films co-doped with sulfur and nitrogen were synthesized using the ultrasonic spray pyrolysis (USP) method to enhance hole concentration through valence band modification. Structural and optical characterizations confirm successful sulfur incorporation and valence band shifting consistent with the valence band anticrossing (VBAC) model. Hall effect measurements reveal a systematic increase in hole concentration with increasing sulfur content.Magnetic and transport measurements indicate a clear correlation between Curie temperature (T C ), carrier density, and resistivity behavior. Notably, resistivity maxima coincide with the ferromagnetic-paramagnetic transition, consistent with the de Gennes-Friedel model of spin-disorder scattering. This observation, along with the systematic enhancement of T C and saturation magnetization with hole concentration, provides compelling evidence of intrinsic carrier-mediated ferromagnetism. These results demonstrate that sulfur-assisted band engineering in ZnO is an effective strategy to modulate magnetic and transport properties in oxide-based DMSs, offering a promising route for future spintronic applications.</jats:p>