skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Suppressing phase disproportionation in quasi-2D perovskite light-emitting diodes
Abstract Electroluminescence efficiencies and stabilities of quasi-two-dimensional halide perovskites are restricted by the formation of multiple-quantum-well structures with broad and uncontrollable phase distributions. Here, we report a ligand design strategy to substantially suppress diffusion-limited phase disproportionation, thereby enabling better phase control. We demonstrate that extending the π-conjugation length and increasing the cross-sectional area of the ligand enables perovskite thin films with dramatically suppressed ion transport, narrowed phase distributions, reduced defect densities, and enhanced radiative recombination efficiencies. Consequently, we achieved efficient and stable deep-red light-emitting diodes with a peak external quantum efficiency of 26.3% (average 22.9% among 70 devices and cross-checked) and a half-life of ~220 and 2.8 h under a constant current density of 0.1 and 12 mA/cm 2 , respectively. Our devices also exhibit wide wavelength tunability and improved spectral and phase stability compared with existing perovskite light-emitting diodes. These discoveries provide critical insights into the molecular design and crystallization kinetics of low-dimensional perovskite semiconductors for light-emitting devices.  more » « less
Award ID(s):
2110706 2110814 2131608
PAR ID:
10416401
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; more » ; ; ; ; ; « less
Date Published:
Journal Name:
Nature Communications
Volume:
14
Issue:
1
ISSN:
2041-1723
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract Metal halide perovskites show promise for next-generation light-emitting diodes, particularly in the near-infrared range, where they outperform organic and quantum-dot counterparts. However, they still fall short of costly III-V semiconductor devices, which achieve external quantum efficiencies above 30% with high brightness. Among several factors, controlling grain growth and nanoscale morphology is crucial for further enhancing device performance. This study presents a grain engineering methodology that combines solvent engineering and heterostructure construction to improve light outcoupling efficiency and defect passivation. Solvent engineering enables precise control over grain size and distribution, increasing light outcoupling to ~40%. Constructing 2D/3D heterostructures with a conjugated cation reduces defect densities and accelerates radiative recombination. The resulting near-infrared perovskite light-emitting diodes achieve a peak external quantum efficiency of 31.4% and demonstrate a maximum brightness of 929 W sr−1m−2. These findings indicate that perovskite light-emitting diodes have potential as cost-effective, high-performance near-infrared light sources for practical applications. 
    more » « less
  2. Metal-halide perovskites, in particular their nanocrystal forms, have emerged as a new generation of light-emitting materials with exceptional optical properties, including narrow emissions covering the whole visible region with high photoluminescence quantum efficiencies of up to near-unity. Remarkable progress has been achieved over the last few years in the areas of materials development and device integration. A variety of synthetic approaches have been established to precisely control the compositions and microstructures of metal-halide perovskite nanocrystals (NCs) with tunable bandgaps and emission colors. The use of metal-halide perovskite NCs as active materials for optoelectronic devices has been extensively explored. Here, we provide a brief overview of recent advances in the development and application of metal-halide perovskite NCs. From color tuning via ion exchange and manipulation of quantum size effects, to stability enhancement via surface passivation, new chemistry for materials development is discussed. In addition, processes in optoelectronic devices based on metal-halide perovskite NCs, in particular, light-emitting diodes and radiation detectors, will be introduced. Opportunities for future research in metal-halide perovskite NCs are provided as well. 
    more » « less
  3. Abstract Metal halide perovskites have witnessed great success in green, red, and near‐infrared light‐emitting diodes (LEDs), yet blue LEDs still lag behind. Reducing undesired energetic disorders – broad n ‐phases and halide segregation – is considered as the most critical strategy to further improve the performances. Here, the study reports a newly designed and synthesized di‐ammonium ligand with rigid π ‐conjugated rings and additional methyl groups to construct Dion–Jacobson (DJ) structure. Augmented coordination from the extra ammonium site and increased effective bulkiness from methyl groups lead to better distribution control over conventional mono‐ammonium ligands. This enhances the radiative recombination of blue emissions in the film with homogeneous energy landscape and improved surface morphology, as evidenced by a series of imaging and mapping techniques. As a result, it demonstrates DJ perovskite LEDs (PeLEDs) with peak external quantum efficiencies of ≈4% at 484 nm and ≈11% at 494 nm, which are among the top reported for pure DJ phase‐based PeLEDs in the corresponding wavelength regions. The results deepen the understanding of regulating energetic disorders in perovskite materials via molecular engineering. 
    more » « less
  4. Perovskite light-emitting diodes (PeLEDs) are advancing because of their superior external quantum efficiencies (EQEs) and color purity. Still, addi-tional work is needed for blue PeLEDs to achieve the same benchmarks as the other visible colors. This study demonstrates an extremely efficient blue PeLED with a 488 nm peak emission, a maximum luminance of 8600 cd m−2, and a maximum EQE of 12.2% by incorporating the double-sided ethane-1,2-diammonium bromide (EDBr2) ligand salt along with the long-chain ligand methylphenylammonium chloride (MeCl). The EDBr2 successfully improves the interaction between 2D perovskite layers by reducing the weak van der Waals interaction and creating a Dion–Jacobson (DJ) structure. Whereas the pristine sample (without EDBr2) is inhibited by small stacking number (n) 2D phases with nonradiative recombination regions that diminish the PeLED performance, adding EDBr2 successfully enables better energy transfer from small n phases to larger n phases. As evidenced by photoluminescence (PL), scanning electron microscopy (SEM), and atomic force microscopy (AFM) characterization, EDBr2 improves the morphology by reduction of pinholes and passivation of defects, subsequently improving the efficiencies and operational lifetimes of quasi-2D blue PeLEDs. 
    more » « less
  5. Because of their enhanced quantum confinement, colloidal two-dimensional Ruddlesden–Popper (RP) perovskite nanosheets with a general formula L 2 [ABX 3 ] n −1 BX 4 stand as a promising narrow-wavelength blue-emitting nanomaterial. Despite ample studies on batch synthesis, for RP perovskites to be broadly applied, continuous synthetic routes are needed. Herein, we design and optimize a flow reactor to continuously produce high-quality n = 1 RP perovskite nanoplatelets. The effects of antisolvent composition, reactor tube length, precursor solution injection rate, and antisolvent injection rate on the morphology and optical properties of the nanoplatelets are systematically examined. Our investigation suggests that flow reactors can be employed to synthesize high-quality L 2 PbX 4 perovskite nanoplatelets ( i.e. , n = 1) at rates greater than 8 times that of batch synthesis. Mass-produced perovskite nanoplatelets promise a variety of potential applications in optoelectronics, including light emitting diodes, photodetectors, and solar cells. 
    more » « less