skip to main content


Title: Highly Efficient Quasi 2D Blue Perovskite Electroluminescence Leveraging a Dual Ligand Composition
Abstract

Perovskite light‐emitting diodes (PeLEDs) are advancing because of their superior external quantum efficiencies (EQEs) and color purity. Still, additional 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 EDBr2successfully 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 EDBr2successfully enables better energy transfer from smallnphases to largernphases. As evidenced by photoluminescence (PL), scanning electron microscopy (SEM), and atomic force microscopy (AFM) characterization, EDBr2improves the morphology by reduction of pinholes and passivation of defects, subsequently improving the efficiencies and operational lifetimes of quasi‐2D blue PeLEDs.

 
more » « less
Award ID(s):
2209871 1906505
NSF-PAR ID:
10405583
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Functional Materials
Volume:
33
Issue:
28
ISSN:
1616-301X
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Blue electroluminescence is highly desired for emerging light‐emitting devices for display applications and optoelectronics in general. However, saturated, efficient, and stable blue emission has been challenging to achieve, particularly in mixed‐halide perovskites, where intrinsic ion motion and halide segregation compromises spectral purity. Here, CsPbBr3−xClxperovskites, polyelectrolytes, and a salt additive are leveraged to demonstrate pure blue emission from single‐layer light‐emitting electrochemical cells (LECs). The electrolytes transport the ions from salt additives, enhancing charge injection and stabilizing the inherent perovskite emissive lattice for highly pure and sustained blue emission. Substituting Cl into CsPbBr3tunes the perovskite luminescence from green through blue. Sky blue and saturated blue devices produce International Commission on Illumination coordinates of (0.105, 0.129) and (0.136, 0.068), respectively, with the latter meeting the US National Television Committee standard for the blue primary. Likewise, maximum luminances of 2900 and 1000 cd m−2, external quantum efficiencies (EQEs) of 4.3% and 3.9%, and luminance half‐lives of 5.7 and 4.9 h are obtained for sky blue and saturated blue devices, respectively. Polymer and LiPF6inclusion increases photoluminescence efficiency, suppresses halide segregation, induces thin‐film smoothness and uniformity, and reduces crystallite size. Overall, these devices show superior performance among blue perovskite light‐emitting diodes (PeLEDs) and general LECs.

     
    more » « less
  2. 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 – broadn‐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 rigidπ‐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
  3. Abstract

    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.

     
    more » « less
  4. Abstract

    Tri‐cation (Cs+/CH3NH3+/CH(NH2)2+) and dual‐anion (Br/I) perovskites are promising light absorbers for inexpensive infrared (IR) photodetectors but degrade under prolonged IR exposure. Here, stable IR photodetectors based on electrospun tri‐cation perovskite fibers infiltrated with hole‐transporting π‐conjugated small molecule 2,2′,7,7′‐tetrakis[N,N‐di(4‐methoxyphenyl)amino]‐9,9‐spirobifluorene (Spiro‐OMeTAD) are demonstrated. These hybrid perovskite photodetectors operate at a low bias of 5 V and exhibit ultra‐high gains with external quantum efficiencies (EQEs) as high as 3009%, decreasing slightly to ≈2770% after 3 months in air. These EQE values are almost ten times larger than those measured for photodetectors comprising bilayer perovskite/Spiro‐OMeTAD films. A high density of charge traps on electrospun fiber surfaces gives rise to a photomultiplication effect in which photogenerated holes can travel through the active layer multiple times before recombining with trapped electrons. Time‐resolved photoluminescence and conductive atomic force microscopy mapping reveal the improved performance of electrospun fibers to originate from the significantly enhanced interfacial surface area between the perovskite and Spiro‐OMeTAD compared to bilayers. As a solution‐based, scalable and continuous method of depositing perovskite layers, electrospinning thus presents a promising strategy for the inexpensive fabrication of high‐performance IR photodetectors for applications ranging from information technology to imaging.

     
    more » « less
  5. Abstract

    Perovskite light‐emitting diodes (PeLEDs) have received great attention for their potential as next‐generation display technology. While remarkable progress has been achieved in green, red, and near‐infrared PeLEDs with external quantum efficiencies (EQEs) exceeding 20%, obtaining high performance blue PeLEDs remains a challenge. Poor charge balance due to large charge injection barriers in blue PeLEDs has been identified as one of the major roadblocks to achieve high efficiency. Here band edge control of perovskite emitting layers for blue PeLEDs with enhanced charge balance and device performance is reported. By using organic spacer cations with different dipole moments, that is, phenethyl ammonium (PEA), methoxy phenethyl ammonium (MePEA), and 4‐fluoro phenethyl ammonium (4FPEA), the band edges of quasi‐2D perovskites are tuned without affecting their band gaps. Detailed characterization and computational studies have confirmed the effect of dipole moment modification to be mostly electrostatic, resulting in changes in the ionization energies of ≈0.45 eV for MePEA and ≈ −0.65 eV for 4FPEA based thin films relative to PEA‐based thin films. With improved charge balance, blue PeLEDs based on MePEA quasi‐2D perovskites show twofold increase of the EQE as compared to the control PEA based devices.

     
    more » « less