Ultrafast Thermodynamic Control for Stable and Efficient Mixed Halide Perovskite Nanocrystals

Low photoluminescence quantum yield (PLQY) and spectra instability, the two most difficult challenges in blue-emitting CsPbBrxCl3-x NCs, have not yet been solved. Quickly controlling the reaction thermodynamics is crucial to enhance crystallinity, thus PLQY and spectra stability, but it has been ignored until now. An ultrafast thermodynamic control (UTC) strategy is designed by utilizing liquid nitrogen to instantaneously freeze the superior crystal lattices of CsPbBrxCl3-x NCs formed at high temperature. The average cooling rate exhibits a 33-fold increase compared to conventional ice-water cooling (from 1.5 to 50 K s(-1)). This UTC can make the reaction thermodynamic energy of the system lower than the threshold very quickly. Therefore, abrupt termination of further crystal growth can be achieved, which also avoids additional nucleation at low temperature. With the assist of defect passivation, the final blue-emitting CsPbBrxCl3-x NCs exhibit an absolute PLQY of 98%, representing the highest value in Pb-based blue perovskites to date. More importantly, they exhibit superior spectra instability. This UTC strategy not only represents a new avenue to synthesize perovskite NCs with excellent crystal quality and ultrahigh PLQY, but also provides a good reference to deal with the recognized bottleneck of spectra instability.