While there has been extensive investigation into modulating quasi‐2D perovskite compositions in light‐emitting diodes (LEDs) for promoting their electroluminescence, very few reports have studied approaches involving enhancement of the energy transfer between quasi‐2D perovskite layers of the film, which plays very important role for achieving high‐performance perovskite LEDs (PeLEDs). In this work, a bifunctional ligand of 4‐(2‐aminoethyl)benzoic acid (ABA) cation is strategically introduced into the perovskite to diminish the weak van der Waals gap between individual perovskite layers for promoting coupled quasi‐2D perovskite layers. In particular, the strengthened interaction between coupled quasi‐2D perovskite layers favors an efficient energy transfer in the perovskite films. The introduced ABA can also simultaneously passivate the perovskite defects by reducing metallic Pb for less nonradiative recombination loss. Benefiting from the advanced properties of ABA incorporated perovskites, highly efficient blue PeLEDs with external quantum efficiency of 10.11% and a very long operational stability of 81.3 min, among the best performing blue quasi‐2D PeLEDs, are achieved. Consequently, this work contributes an effective approach for high‐performance and stable blue PeLEDs toward practical applications.
Quasi‐2D Ruddlesden–Popper halide perovskites with a large exciton binding energy, self‐assembled quantum wells, and high quantum yield draw attention for optoelectronic device applications. Thin films of these quasi‐2D perovskites consist of a mixture of domains having different dimensionality, allowing energy funneling from lower‐dimensional nanosheets (high‐bandgap domains) to 3D nanocrystals (low‐bandgap domains). High‐quality quasi‐2D perovskite (PEA)2(FA)3Pb4Br13films are fabricated by solution engineering. Grazing‐incidence wide‐angle X‐ray scattering measurements are conducted to study the crystal orientation, and transient absorption spectroscopy measurements are conducted to study the charge‐carrier dynamics. These data show that highly oriented 2D crystal films have a faster energy transfer from the high‐bandgap domains to the low‐bandgap domains (<0.5 ps) compared to the randomly oriented films. High‐performance light‐emitting diodes can be realized with these highly oriented 2D films. Finally, amplified spontaneous emission with a low threshold 4.16 µJ cm−2is achieved and distributed feedback lasers are also demonstrated. These results show that it is important to control the morphology of the quasi‐2D films to achieve efficient energy transfer, which is a critical requirement for light‐emitting devices.
more » « less- Award ID(s):
- 1729383
- NSF-PAR ID:
- 10457481
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 32
- Issue:
- 16
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Hybrid halide 2D perovskites deserve special attention because they exhibit superior environmental stability compared with their 3D analogs. The closer interlayer distance discovered in 2D Dion–Jacobson (DJ) type of halide perovskites relative to 2D Ruddlesden–Popper (RP) perovskites implies better carrier charge transport and superior performance in solar cells. Here, the structure and properties of 2D DJ perovskites employing 3‐(aminomethyl)piperidinium (3AMP2+) as the spacing cation and a mixture of methylammonium (MA+) and formamidinium (FA+) cations in the perovskite cages are presented. Using single‐crystal X‐ray crystallography, it is found that the mixed‐cation (3AMP)(MA0.75FA0.25)3Pb4I13perovskite has a narrower bandgap, less distorted inorganic framework, and larger PbIPb angles than the single‐cation (3AMP)(MA)3Pb4I13. Furthermore, the (3AMP)(MA0.75FA0.25)3Pb4I13films made by a solvent‐engineering method with a small amount of hydriodic acid have a much better film morphology and crystalline quality and more preferred perpendicular orientation. As a result, the (3AMP)(MA0.75FA0.25)3Pb4I13‐based solar cells exhibit a champion power conversion efficiency of 12.04% with a high fill factor of 81.04% and a 50% average efficiency improvement compared to the pristine (3AMP)(MA)3Pb4I13cells. Most importantly, the 2D DJ 3AMP‐based perovskite films and devices show better air and light stability than the 2D RP butylammonium‐based perovskites and their 3D analogs.
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