Wide-Bandgap Perovskite Quantum Dots in Perovskite Matrix for Sky-Blue Light-Emitting Diodes.
Yuan LiuZiliang LiJian XuYitong DongBin ChenSo Min ParkDongxin MaSeungjin LeeJianan Erick HuangSam TealeOleksandr VoznyyEdward H SargentPublished in: Journal of the American Chemical Society (2022)
The epitaxial growth of a perovskite matrix on quantum dots (QDs) has enabled the emergence of efficient red light-emitting diodes (LEDs) because it unites efficient charge transport with strong surface passivation. However, the synthesis of wide-band gap ( E g ) QD-in-matrix heterostructures has so far remained elusive in the case of sky-blue LEDs. Here, we developed CsPbBr 3 QD-in-perovskite matrix solids that enable high luminescent efficiency and spectral stability with an optical E g of over 2.6 eV. We screened alloy candidates that modulate the perovskite E g and allow heteroepitaxy, seeking to implement lattice-matched type-I band alignment. Specifically, we introduced a CsPb 1- x Sr x Br 3 matrix, in which alloying with Sr 2+ increased the E g of the perovskite and minimized lattice mismatch. We then developed an approach to passivation that would overcome the hygroscopic nature of Sr 2+ . We found that bis (4-fluorophenyl)phenylphosphine oxide strongly coordinates with Sr 2+ and provides steric hindrance to block H 2 O, a finding obtained by combining molecular dynamics simulations with experimental results. The resulting QD-in-matrix solids exhibit enhanced air- and photo-stability with efficient charge transport from the matrix to the QDs. LEDs made from this material exhibit an external quantum efficiency of 13.8% and a brightness exceeding 6000 cd m -2 .