Metallic transition-metal oxides undergo a metal-to-insulator transition (MIT) as the film thickness decreases across a critical thickness of several monolayers (MLs), but its driving mechanism remains controversial. We have studied the thickness-dependent MIT of the ferromagnetic metal La0.6Sr0.4MnO3 by x-ray absorption
spectroscopy and x-ray magnetic circular dichroism. As the film thickness was decreased across the critical thickness of the MIT (6–8 ML), a gradual decrease of the ferromagnetic signals and a concomitant increase of paramagnetic signals were observed, while theMn valence abruptly decreased towardsMn3+. These observations suggest that the ferromagnetic phase gradually and most likely inhomogeneously turns into the paramagnetic phase and both phases abruptly become insulating at the critical thickness.