skip to main content

Attention:

The NSF Public Access Repository (PAR) system and access will be unavailable from 8:00 PM ET on Friday, March 21 until 8:00 AM ET on Saturday, March 22 due to maintenance. We apologize for the inconvenience.


Title: Efficient Energy Funneling in Quasi‐2D Perovskites: From Light Emission to Lasing
Abstract

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
PAR ID:
10457481
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  
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
More Like this
  1. 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
  2. Abstract

    Following the rejuvenation of 3D organic–inorganic hybrid perovskites, like CH3NH3PbI3, (quasi)‐2D Ruddlesden–Popper soft halide perovskites R2An−1PbnX3n+1have recently become another focus in the optoelectronic and photovoltaic device community. Although quasi‐2D perovskites were first introduced to stabilize optoelectronic/photovoltaic devices against moisture, more interesting properties and device applications, such as solar cells, light‐emitting diodes, white‐light emitters, lasers, and polaritonic emission, have followed. While delicate engineering design has pushed the performance of various devices forward remarkably, understanding of the fundamental properties, especially the charge‐transfer process, electron–phonon interactions, and the growth mechanism in (quasi)‐2D halide perovskites, remains limited and even controversial. Here, after reviewing the current understanding and the nexus between optoelectronic/photovoltaic properties of 2D and 3D halide perovskites, the growth mechanisms, charge‐transfer processes, vibrational properties, and electron–phonon interactions of soft halide perovskites, mainly in quasi‐2D systems, are discussed. It is suggested that single‐crystal‐based studies are needed to deepen the understanding of the aforementioned fundamental properties, and will eventually contribute to device performance.

     
    more » « less
  3. Abstract

    Perovskite light‐emitting diodes (LEDs) have recently attracted great research interest for their narrow emissions and solution processability. Remarkable progress has been achieved in green perovskite LEDs in recent years, but not blue or red ones. Here, highly efficient and spectrally stable red perovskite LEDs with quasi‐2D perovskite/poly(ethylene oxide) (PEO) composite thin films as the light‐emitting layer are reported. By controlling the molar ratios of organic salt (benzylammonium iodide) to inorganic salts (cesium iodide and lead iodide), luminescent quasi‐2D perovskite thin films are obtained with tunable emission colors from red to deep red. The perovskite/polymer composite approach enables quasi‐2D perovskite/PEO composite thin films to possess much higher photoluminescence quantum efficiencies and smoothness than their neat quasi‐2D perovskite counterparts. Electrically driven LEDs with emissions peaked at 638, 664, 680, and 690 nm have been fabricated to exhibit high brightness and external quantum efficiencies (EQEs). For instance, the perovskite LED with an emission peaked at 680 nm exhibits a brightness of 1392 cd m−2and an EQE of 6.23%. Moreover, exceptional electroluminescence spectral stability under continuous device operation has been achieved for these red perovskite LEDs.

     
    more » « less
  4. 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 PbIPb 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.

     
    more » « less
  5. Abstract

    Mixtures of Ce‐doped rare‐earth aluminum perovskites are drawing a significant amount of attention as potential scintillating devices. However, the synthesis of complex perovskite systems leads to many challenges. Designing the A‐site cations with an equiatomic ratio allows for the stabilization of a single‐crystal phase driven by an entropic regime. This work describes the synthesis of a highly epitaxial thin film of configurationally disordered rare‐earth aluminum perovskite oxide (La0.2Lu0.2Y0.2Gd0.2Ce0.2)AlO3and characterizes the structural and optical properties. The thin films exhibit three equivalent epitaxial domains having an orthorhombic structure resulting from monoclinic distortion of the perovskite cubic cell. An excitation of 286.5 nm from Gd3+and energy transfer to Ce3+with 405 nm emission are observed, which represents the potential for high‐energy conversion. These experimental results also offer the pathway to tunable optical properties of high‐entropy rare‐earth epitaxial perovskite films for a range of applications.

     
    more » « less