Perovskite-based optoelectronic devices are gaining much attention owing to their remarkable performance and low processing cost, particularly for solar cells. However, for perovskite light-emitting diodes, non-radiative charge recombination has limited the electroluminescence efficiency. Here we demonstrate perovskite–polymer bulk heterostructure light-emitting diodes exhibiting external quantum efficiencies of up to 20.1% (at current densities of 0.1–1 mA cm⁻²). The light-emitting diode emissive layer comprises quasi-two-dimensional and three-dimensional (2D/3D) perovskites and an insulating polymer. Photogenerated excitations migrate from quasi-2D to lower-energy sites within 1 ps, followed by radiative bimolecular recombination in the 3D regions. From near-unity external photoluminescence quantum efficiencies and transient kinetics of the emissive layer with and without charge-transport contacts, we find non-radiative recombination pathways to be effectively eliminated, consistent with optical models giving near 100% internal quantum efficiencies. Although the device brightness and stability (T₅₀ = 46 h in air at peak external quantum efficiency) require further improvement, our results indicate the significant potential of perovskite-based photon sources.

基于钙钛矿的光电器件由于其卓越的性能和较低的处理成本而受到了广泛的关注，特别是对于太阳能电池而言。然而，对于钙钛矿发光二极管，非辐射电荷复合限制了电致发光效率。在这里，我们演示了钙钛矿聚合物整体异质结构发光二极管，其外部量子效率高达20.1％（在电流密度为0.1–1 mA cm ^{-2的情况下）}）。发光二极管发光层包括准二维和三维（2D / 3D）钙钛矿和绝缘聚合物。光生激发在1 ps内从准2D迁移到较低能量的位点，然后在3D区域进行辐射性双分子重组。从近统一的外部光致发光量子效率和带有或不带有电荷传输接触的发光层的瞬态动力学，我们发现非辐射复合途径被有效消除，这与光学模型相符，具有接近100％的内部量子效率。尽管器件的亮度和稳定性（ 在外部量子效率达到峰值时在空气中的T ₅₀ = 46 h）需要进一步改善，但我们的结果表明，钙钛矿基光子源具有巨大潜力。