Abstract
1. Introduction
The halide perovskite is a promising material with ABX3 formation and perovskite structure. A monovalent cation is used in the A-site; methyl ammonium (MA), formamidinium (FA), Rb, and Cs. For the B-site, divalent metal, typically Pb, is used. For X site, halides are used; I, Br, and Cl. These halide perovskites attracted many researchers with fascinating properties, such as high charge carrier mobility[
The perovskite LEDs (PeLEDs) have been expected to be the leading candidate for the next generation displays due to narrower emission spectrum than other materials, and the PeLEDs have been rapidly developed in past few years with intensive research. The external quantum efficiency (EQE) of the PeLEDs have been enhanced from below 1% to over 20% for green and red colors[
This review introduces the recent progress of the blue PeLEDs first, which focuses on the development of emissive layers. The emissive layer is categorized into three groups, perovskite nanocrystals (PeNCs), 2-dimensional (2D) and quasi-2D perovskites, and bulk (3D) perovskites. Subsequently, the developments of interlayers and interfacial engineering methods will be discussed secondly. Next, we discuss the remaining huddles in blue PeLEDs such as performance limitations, device instability issues, and presents perspective of the blue PeLEDs.
2. Developments in emissive layer
2.1. PeLEDs with perovskite nanocrystals (PeNCs)
2.1.1. Synthesis methods of blue emissive PeNCs
The halide perovskite nanocrystals (PeNCs) are nanometer-sized perovskite crystals, wrapped with organic ligands. By the organic ligands, the PeNCs are dispersed in organic solvents. The presence of organic ligands increases the exciton binding energy of the PeNCs, because electrically insulating ligands confine the charge transport behavior. Increased exciton binding energy enhance radiative recombination rates, and this is the main reason of most of PeNCs shows higher PLQY results than other types of perovskites. Unlike two other types of perovskites, the 2D perovskites and bulk (3D) perovskites, the PeNCs must be synthesized before fabrication of emissive layers. The first synthesis of PeNCs was reported by Schmidt et al.[
The general synthesis method of the PeNCs is based on the hot-injection method, which is well known and widely using method in the quantum dot fields[
A common synthesis process of blue emissive PeNCs is injecting Cs precursors into the PbBr2, PbCl2, and organic ligand mixed precursors at high injection temperature[
Figure 1.(Color online) Synthesis and engineering methods of PeNCs to improve the performance of the blue PeLEDs. Schematic diagrams of synthesis method of the blue emissive PeNCs through (a) hot injection method, (b) LARP method[
The LARP method is simpler than the hot-injection method for obtaining the PeNCs. When perovskite precursors and organic ligand mixed solution is added into nonpolar solvent, nanometer-size perovskite crystals are immediately synthesized[
After the PeNCs synthesis, the halide ratio in the PeNCs could be tuned more to obtain blue emissive PeNCs[
2.1.2. PeLEDs with PeNCs
The first blue PeLEDs based on the PeNCs were produced by Song et al. with CsPb(Br/Cl)3 PeNCs[
The basic purpose of these ligand exchanging techniques is removing original ligands such as oleic acids or oleylamines. These common ligands are easy to handle and provide good colloidal stability with long alkyl chain, however, become a barrier to charge carrier injection. Therefore, exchanging ligands should have shorter alkyl chain to improve the charge carrier injection. In a similar vein, the ligand density in PeNCs could also be a considerable factor in the performance of blue PeLEDs[
Another main strategy to increase the luminescence efficiency of PeNCs is the halide defect passivation. The halide defects are a major factor that creates trap-states in electronic band of the PeNCs and lowers radiative recombination in the PeNCs. Therefore, removing the halide defects is an efficient way to improve the PeLEDs and lots of methods were proposed[
Recently, Dong et al. reported surface engineering method on CsPbBr3 quantum dots for blue PeLEDs[
2.2. PeLEDs with 2-dimensional (2D) and quasi-2D perovskites
2D perovskites and quasi-2D perovskites have formation of R2An–1BnX3n+1, where R is an aryl or alkyl group, and n value represents the number of layers of perovskite crystals. Considering that n = 1 is 2D perovskite and n = ∞ is 3D perovskite, the perovskites with the n value bigger than 1 called as quasi-2D perovskites (Fig. 2(a)). These 2D and quasi-2D perovskites are formed with the assistance of organic spacing molecules, and importantly, the number of perovskite layers are tuned by selection of the organic spacing molecules and by controlling the condition of those molecules. For ideal case (n = 1), the 2D perovskite could be expressed as (R-NH3)2BX4, also known as the Ruddlesden-Popper perovskite[
Figure 2.(Color online) (a) Schematic diagrams of the Ruddlesden-Popper perovskite and quasi-2D perovskites[
The emissive layers with quasi-2D perovskites have less organic spacing molecules in the film, resulted with improved optoelectronic properties by reduced exciton-phonon coupling. Additionally, the quasi-2D perovskites form an efficient energy level structure. When a quasi-2D perovskites are formed, the film usually has a mixed phase state with several n values, not a uniform phase with a single n value. This mixed phase state naturally constructs energy funnel structure that provides better charge transport, higher radiative recombination chances, and improved device performance[
Kumar et al. proposed a blue PeLEDs with quasi-2D perovskite that have formation of OLA2MAn–1PbnBr3n+1, where n = 3–5 and OLA = oleylammonium[
The blue PeLEDs with quasi-2D perovskite with single halide composition, Br, have intensively been studied due to easy of fabrication, free from the halide segregation ensuring stable color spectra (Fig. 2(e)), and excellent performances. However, most of quasi-2D perovskites exhibited sky-blue color, at around 490 nm emission peak. One of the main reasons for the sky-blue color result is that it is hard to obtain pure single phase quasi-2D perovskites with low n value through solution process. The emission spectra of quasi-2D perovskites at mixed phase state is determined by the largest n value in the film. Therefore, if the film could not have pure phases with low n value, which is hard to achieve, the emissive layer could not exhibit the pure blue color emission. Additionally, as the emission peak of the quasi-2D perovskites is not continuous with n values, it is also hard to obtain desired specific emission peak at around 470 nm. Therefore, obtaining pure blue color PeLEDs around 470 nm with quasi-2D perovskites with a single halide composition is difficult. Moreover, the emission spectra from single halide quasi-2D perovskite films have shown broader or multiple emission peaks that reduces great advantages of the PeLEDs, by uncontrolled radiative recombination from the mixed phases in the films. Several attempts were conducted to obtain pure blue emission spectra with quasi-2D perovskites, with participation of Cl elements[
2.3. PeLEDs with bulk (3D) perovskites
Low-dimensional perovskites have alternative way to obtain blue emission with assistance of the quantum confinement effect, and the properties can be enhanced by organic molecules. However, it is inevitable to use Cl element to achieve the blue emission with bulk perovskites, which is the biggest problem to obtain highly efficient blue PeLEDs. The inorganic Cl precursors are rarely solved in most of solvents, which leads poor film morphology resulting limited performances (Fig. 3(a)). Fortunately, Cl precursors with organic counter cations have better solubility and demonstrated the potential of bulk perovskites for blue PeLEDs.
Figure 3.(Color online) (a) Surface images of bulk (3D) perovskite with varying Cl contents in the film and (b) corresponding PL spectra of bulk perovskites[
The first blue PeLEDs with bulk perovskite was reported by Kumawat et al. with MAPb(Br1–xClx)3 (x = 0–1), with clear blue color emission[
Producing emissive layers through mixed A-site cations could be an effective way to obtain high-quality films. By mixing the A-site cations, the formation energy of the perovskite could be increased, the defect density in the perovskite crystals could be reduced, and the device performance could be enhanced. Moreover, with reduced defect density, the halide segregation could be reduced to have better spectral stability (Figs. 3(c) and 3(d)). Kim et al. used three types of cations (Cs, MA, FA) for bulk perovskites and successfully fabricated blue PeLEDs with EQE of 1.7% at 475 nm emission peak[
Though mixing cation is effective strategy to improve the performance of the blue PeLEDs, the bulk perovskites with organic cations have some problems that moisture absorbing properties of organic cation combined Cl precursors, and resulted with high defect density in the pure blue color PeLEDs. However, the inorganic bulk perovskites for blue PeLEDs are much more difficult to fabricate due to even lower solubility of inorganic Cl sources. To solve the problem of insoluble Cl precursors, alternative ways to get wide optical bandgap were tried. Wang et al. reported that introducing the Rb cations into the Cs based perovskite causes lattice distortion and widens the optical bandgap[
The bulk perovskites have disadvantages such as difficulties in film morphology, exciton quenching between charge transport layers and emissive layer due to lack of electronic band confining organic molecules, and halide segregations. However, the bulk perovskites have advantages on cheap precursors, simpler fabrication methods, stable to most of non-polar solvents which enables fabricating organic layers on top of emissive layers by solution processing methods. In addition, the bulk perovskites are free from the charge blocking organic molecules, the bulk perovskite could have better maximum luminance with higher current injection when the material quality and stability are guaranteed.
3. Developments in charge transport/ injection layers
3.1. Hole transport/ injection layers (HTL/HIL)
With excellent wetting property to form all three types of perovskite emissive layers, poly(3,4-ethylenedioxythiophene): polystyrenesulfonate) (PEDOT:PSS) is widely used for blue PeLEDs, and the p–i–n structure that using PEDOT:PSS as a substrate is common structure for the blue PeLEDs. However, due to the deep valence band maximum of blue emissive perovskites and shallow HOMO (highest occupied molecular orbital) of the PEDOT:PSS, there is a large energy barrier to inject holes from PEDOT:PSS layer to the emissive perovskite layers. Moreover, the acidic property of the PEDOT:PSS layer could be potential origin of degradation of devices. Therefore, to match the energy levels with emissive layer, to improve the charge injection, to match the charge injection balance, and to enhance the device stability, various genuine HTL/HIL materials and related engineering techniques to improve the properties of HTL/HIL were suggested for all three types of blue emissive perovskite materials (Fig. 4(a)).
Figure 4.(Color online) (a) Energy levels of various charge transport/ injection layer materials with blue emissive perovskite. (b) TFB/PFI bilayer structure strategy to reduce hole injection barrier[
Jang et al. improved wettability, compatibility of PEDOT:PSS, which results better perovskite crystal growth process, with assistance of conjugate polyelectrolytes (CPEs)[
However, the polymeric HTL/HIL could disturb perovskite crystal growth due to low wettability of precursor solutions in polar solvents for the bulk perovskites. Considering the disadvantages of organic HTL/HIL, the inorganic oxide HTL/HIL could be promising HTL/HIL for the bulk blue LEDs[
3.2. Electron transport/ injection layers (ETL/EIL)
As the p–i–n structure is common structure in the blue PeLEDs field, usually the ETL/EIL are fabricated upon the blue emissive perovskite layers. The main problem is that the perovskite layers have weak chemical stability and are easily decomposed with polar solvents, making difficult to fabricate ETL/EIL with solution processing methods. Therefore, most of the ETL/EIL for blue PeLEDs are formed through a thermal evaporation method, which is a difficult method to control the chemical properties of the materials. In addition, most of the ETL/EIL materials used for blue PeLEDs already have shallower energy level than perovskite materials (Fig. 4(a)), so the bottle neck of charge injection is HTL/HIL usually. As a result, not many approaches have been reported to make significant changes to control the properties of the ETL/EIL materials itself for blue PeLEDs.
For the n–i–p structure, perovskite emissive layers are fabricated onto the ETL/EIL. Because most known ETL/EIL materials are organic materials that disturb the use of polar solvents due to poor wetting properties, bulk perovskites are almost impossible to fabricate onto the organic ETL/EIL materials. However, the PeNCs or the quasi-2D perovskite emissive layers already have PEDOT:PSS material that has superior wetting properties for the p-i-n structure. Therefore, only a few n–i–p structure based PeLEDs with bulk perovskites were tested with oxide ETL/EIL materials[
3.3. Recombination zone control
It is obvious that the electron and hole transport/injection behavior should be carefully controlled to recombine with each other in the proposed recombination zone, the emissive perovskite layers, as well as to balance the charge carrier injection. However, as the perovskite emissive layers are very thin, less than few tens of nanometers, the charge carriers could be recombined not at the emissive layer but at the adjacent interlayers. Generally, the position of the recombination zone could be controlled by adjusting the thickness of interlayers[
Additionally, introducing a very thin insulating materials between the interlayers and the emissive layers could support the charge carriers to recombine at the emissive perovskite layers. The thin insulating layers allow charge injection by tunnelling effect and provide energy barrier to prevent the leakage of holes to ETL/EIL or electrons to HTL/HIL[
4. Remaining challenges
4.1. Quantum efficiency of emissive layers
The EQE of the PeLEDs is determined by internal quantum efficiency (IQE) and the outcoupling efficiency of the device. The IQE is the product of charge carrier balance, the fraction of excitons capable of radiative decay, and the effective radiative quantum yield[
For PeNCs, surface defects are the main cause of trap states that lowers the effective radiative recombination. The common ligands, oleic acids and/or oleylamines, could be easily detached with purification process or environmental reasons, so exchanging these ligands to the ligands that make stronger bond is effective way to prevent and passivate the surface defects of PeNCs. For now, various ligands, such as ligands that have secondary amines[
For 2D and quasi-2D perovskites, various successful defect engineering techniques were reported[
Hopefully, attempts to reduce the defect and trap states in the emissive layers have shown successful results with improved PLQY of emissive layers reaching near unity value, and enhanced EQE of the blue PeLEDs. However, despite the extremely high PLQY values, the device performance of the blue PeLEDs remained at around over 10% of EQE. Considering the other color PeLEDs resulted around 25% of EQE which is reaching the theoretical limits, it seems there is still some room for improving the performance of the blue PeLEDs. Assuming the emissive layers are perfect, to improve the device performance, the interlayers should be seriously discussed. The common trend of improving the device performance through interlayer engineering was dealing with the HTL/HIL because the HTL/HIL have inferior carrier transport/injection behavior than the ETL/EIL due to charge injection barriers. Fortunately, many successful attempts on the HTL/HIL improved charge carrier transport/ injection properties, reaching that of commonly used ETL/EIL to balance the charge carrier injection. To achieve the theoretical limit of EQE with blue PeLEDs, it is time to develop ETL/EIL materials to have superior charge transport/ injection behavior than conventional materials, and for HTL/HIL too. From simple strategies to modify the interfaces to have better electronic band structure to synthesizing innovative materials should be conducted to reach extremely efficient blue PeLEDs.
4.2. Operational stability and color stability
The low formation energy is a great advantage of halide perovskites, enabling formation of highly crystalline films with solution processing at room temperature condition. However, the low formation energy has another aspect. The low formation energy causes easy and frequent creation of ionic defects which eventually deform and damage the perovskite crystals. These ionic defects sites not only serve as the non-radiative recombination centers, but also impede material stability and operational stability of PeLEDs[
However, state-of-art mixing A-site technique requires many A-site cations[
Another big remaining problem that must be solved is color instability. The main cause of this color instability comes from the mobile characteristic of halides in the halide perovskite crystals[
However, no matter how well the perovskite composition is controlled, it is impossible to permanently prevent the halide segregation with mixed halide compositions, because the halide segregation strongly affected by uncontrollable entropic factors. Fortunately, we already know the perfect method to prevent the halide segregation, that forming the perovskite with a single halide, Br. Though the Br only perovskites need additional delicate size control to get quantum confinement effect to exhibit blue color emission, but at least there are lots of methods and possibilities to broaden the bandgap for Br only perovskites, while it is almost impossible to prevent the halide segregation with mixed halide perovskites.
5. Conclusions and outlook
We introduced recent developments in the blue PeLEDs (Table 1) and remaining challenges, low quantum efficiency of emissive materials and device instability. With the deep understand of material characteristics, the blue PeLEDs showed dramatic developments in past few years. To improve device performance, the strategy of increasing the formation energy through mixing A-site cations have been effective way for all three types of perovskites. Reducing Cl contents in the perovskite material and reducing the size of the perovskite crystal could be effective method to obtain efficient and color stable emissive perovskite layer for sky-blue PeLEDs. For the pure blue PeLEDs with narrow emission spectra, the participation of the Cl element seems inevitable for now, so to realize the highly efficient pure blue PeLEDs, the halide defect engineering technique is essential to handle the trap states in the mixed halide perovskites. However, the Cl element should eventually be eliminated to avoid halide segregation and to get enhanced color stability for pure blue PeLEDs in future. Additionally, advanced interfacial engineering techniques and innovative materials for interlayers should be developed to improve charge carrier injection and to reach the theoretical performance limit. With improved performance and long-term device stability, the blue perovskite LEDs will be the best choice for next generation displays.
Acknowledgements
This work was supported by "the Research Project Funded by U-K Brand" (1.210037.01, 1.200041.01) of UNIST(Ulsan National Institute of Science & Technology). This work was supported by Nano Material Technology Development Program through the National Research Foundation of Korea (NRF) funded by Ministry of Science and ICT (NRF-2021M3H4A1A02049634).
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