Ali, N.Singh, B.A R, V.Lal, S.Yadav, C.S.Tarafder, K.Ghosh, S.2026-02-052021Journal of Physical Chemistry C, 2021, 125, 14, pp. 7734-774519327447https://doi.org/10.1021/acs.jpcc.0c08407https://idr.nitk.ac.in/handle/123456789/23256We present a joint theoretical and experimental investigation on the origin of ferromagnetism in Mn-doped ZnO. Theoretical calculations revealed that the zinc vacancy (VZn) induces ferromagnetic ordering (FMO), whereas the oxygen vacancy (VO) quenches FMO in the Mn-doped ZnO system. This is further corroborated by the experimental results. Magnetic measurements revealed that Mn-doped ZnO shows room-temperature ferromagnetism (RTFM). Saturated magnetic moment per Mn2+ ion increases with oxygen partial pressure, indicating that the VZn enhances FMO in Mn-doped ZnO. Electron paramagnetic resonance and photoluminescence measurements revealed the presence of VZn in Mn-doped ZnO films. X-ray photoelectron spectroscopy measurements showed mixed oxidation states of Mn in Mn-doped ZnO films. Finally, we show that RTFM at very low doping concentrations is due to the overlapping of bound magnetic polarons. However, due to antiferromagnetic coupling at higher doping concentrations, the FMO weakens. © 2021 American Chemical Society.AntiferromagnetismBinary alloysII-VI semiconductorsMagnetic momentsManganese metallographyMetallic filmsOxide mineralsOxygenParamagnetic resonancePolaronsSemiconductor dopingX ray photoelectron spectroscopyZinc oxideAntiferromagnetic couplingExperimental investigationsFerromagnetic orderingsLow doping concentrationsOxygen partial pressurePhotoluminescence measurementsRoom temperature ferromagnetism (RTFM)Theoretical calculationsFerromagnetism