The KNN rollercoaster: from bulk ceramics to phase engineered wafer-scale thin films
Since the initial disclosure of the extraordinary piezoelectric coefficients of Potassium sodium niobate (KNN) in near-equimolar bulk ceramics, its development trajectory has resembled a rollercoaster, with its integration into microelectronics severely lagging due to thermodynamic stability issues and poor planar process compatibility. In this work, we revisit the bulk-derived phase diagram for the specific case of thin films integrated on silicon. By systematically investigating Mn-doped K1-xNaxNbO3 films grown on 8-inch wafers, we demonstrate that the optimal stoichiometry for thin films fundamentally diverges from the bulk equimolar standard. A Na-rich composition (> 70 at.%) is required to overcome substrate-induced constraints, effectively suppressing pyrochlore formation and chemical phase segregation while promoting dense columnar growth with a complete (001) out-of-plane polar orientation. Consequently, Na-rich films deliver outstanding functional properties, reaching remanent polarizations up to 14 uC cm-2, with piezoelectric coefficients of d33f= 79 pm/V and e31f = 10 C/m2. Supported by Density Functional Theory simulations, we correlate this enhancement with improved stability and a strain-driven structural reorientation toward a lower-symmetry monoclinic phase with tilted polarization. By redefining the phase engineering rules for wafer-scale thin films, our results establish a clear route toward KNN integration in microsystems.