Lewis Base Plays a Double-Edged-Sword Role in Trap State Engineering of Perovskite Polycrystals

We report the double-edged-sword effect of the thiourea (a typical Lewis base) additive for tailoring the trap state distribution of perovskite polycrystalline films. Through the thiourea treatment, the polycrystal grain size is greatly increased because of the reduced crystallization activation energy, which, together with the surface defect passivation, alters the density of the energetically "deep" and "shallow" trap states in a trade-off manner. Based on this finding and further photoelectric and spectral studies, the nonmonotonic dependence of the photoluminescence intensity on the thiourea concentration and the complicated time-resolved photoluminescence behavior are excellently clarified. As a proof of concept, the photophysical performance of perovskite polycrystals is optimized via a modified Lewis base treatment by taking the proposed double-edged-sword effect into account.