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Abstract:

Mixed-halide perovskites offer bandgap tunability essential for multijunction solar cells; however, a detrimental halide segregation under light is often observed. Here we combine simultaneous in situ photoluminescence and X-ray diffraction measurements to demonstrate clear differences in compositional and optoelectronic changes associated with halide segregation in MAPb(Br_0.5I_0.5)₃ and FA_0.83Cs_0.17Pb(Br_0.4I_0.6)₃ films. We report evidence for low-barrier ionic pathways in MAPb(Br_0.5I_0.5)₃, which allow for the rearrangement of halide ions in localized volumes of perovskite without significant compositional changes to the bulk material. In contrast, FA_0.83Cs_0.17Pb(Br_0.4I_0.6)₃ lacks such low-barrier ionic pathways and is, consequently, more stable against halide segregation. However, under prolonged illumination, it exhibits a considerable ionic rearrangement throughout the bulk material, which may be triggered by an initial demixing of A-site cations, altering the composition of the bulk perovskite and reducing its stability against halide segregation. Our work elucidates links between composition, ionic pathways, and halide segregation, and it facilitates the future engineering of phase-stable mixed-halide perovskites.

Abstract:

Lead-based halide perovskites have received great attention in light-emitting applications due to their excellent properties, including high photoluminescence quantum yield (PLQY), tunable emission wavelength, and facile solution preparation. In spite of excellent characteristics, the presence of toxic element lead directly obstructs their further commercial development. Hence, exploiting lead-free halide perovskite materials with superior properties is urgent and necessary. In this review, the deep-seated reasons that benefit light emission for halide perovskites, which help to develop lead-free halide perovskites with excellent performance, are first emphasized. Recent advances in lead-free halide perovskite materials (single crystals, thin films, and nanocrystals with different dimensionalities) from synthesis, crystal structures, optical and optoelectronic properties to applications are then systematically summarized. In particular, phosphor-converted LEDs and electroluminescent LEDs using lead-free halide perovskites are fully examined. Ultimately, based on current development of lead-free halide perovskites, the future directions of lead-free halide perovskites in terms of materials and light-emitting devices are discussed.

Abstract:

Light-emitting devices (LEDs) with inorganic perovskite nanocrystals (PNCs) fabricated through the all-solution process have tremendous potential for new-generation illumination and displays on account of their large area and cost-effective manufacturing. However, the development of efficient solution-processed PNC LEDs remains challenge, which mainly results from the fact that only a few types of charge transport layers can be employed for the subsequent deposition steps, thus leading to injection barriers and charge injection imbalance inside these LEDs. Herein 4,4'-bis(carbazole-9-yl) biphenyl (CBP) is introduced as a dopant into the poly(9,9-dioctylfluorene-co-N-(4-(3-methylpropyl)) diphenylamine) (TFB) hole transport layer (HTL), which efficiently modulates the mobility of charge carrier as well as the energy level of the HTL, resulting in the barrier-free injection of the charge carrier in the as-fabricated solution-processed PNC LEDs. Consequently, the luminance of red LEDs (688 nm) reaches 2990 cd m^-2, and the external quantum efficiency achieves 8.1%, which is the optimal performance for solution-processed PNC LEDs to date. Additionally, the turn-on voltage and roll-off have also been improved by the more balanced charge injection.