LAUSR

The density layering phenomenon originating from a free surface gives rise to the layerlike dynamics and stress heterogeneity in ultrathin Cu-Zr glassy films, which facilitates the occurrence of multistep relaxations in the timescale of computer simulations. Taking advantage of this condition, we trace the relaxation decoupling and evolution with temperature simply via the intermediate scattering function. We show that the β relaxation hierarchically follows fast and slow modes in films, and there is a β-relaxation transition as the film is cooled close to the glass transition. We provide the direct observation of particle motions responsible for the β relaxation and reveal the dominant mechanism varying from the thermal activated to the cooperative jumps across the transition.