Surface Treatment with Tailored π-Conjugated Fluorene Derivatives Significantly Enhances the Performance of Perovskite Light-Emitting Diodes.

Surface defect passivation and carrier injection regulation have emerged as effective strategies for enhancing the performance of perovskite light-emitting diodes (Pero-LEDs). It usually requires two functional molecules to realize defect passivation and carrier injection regulation separately. In other words, developing one single molecule possessing these capabilities remains challenging. Herein, we utilized π-conjugated fluorene derivatives as surface treatment materials, 9,9-Spirobi[fluorene] (SBF), 9,9-Spirobifluoren-2-yl-diphenylphosphine oxide (SPPO1), and 2,7-bis(diphenylphosphoryl)-9,9'-spirobifluorene (SPPO13), to investigate the influence of their chemical structure on device optoelectronic performance, especially for defect passivation and carrier injection regulation. Consequently, the passivation capability of double-bonded SPPO13 surpassed single-bonded SPPO1 and nonbonded SBF, which all showed excellent electron transport properties, enhancing electron injection. The maximum external quantum efficiencies (EQE) for Pero-LEDs treated with SBF, SPPO1, and SPPO13 were 8.13, 17.48, and 22.10%, respectively, exceeding that of the derivative-free device (6.55%). Notably, SPPO13-treated devices exhibited exceptional reproducibility, yielding an average EQE of 20.00 ± 1.10% based on 30 devices. This result emphasizes the potential of tailored fluorene derivatives for enhancing the device performance of Pero-LEDs.