Flexible perovskite light-emitting diodes for display applications and beyond

The flexible perovskite light-emitting diodes(FPeLEDs),which can be expediently integrated to portable and wearable devices,have shown great potential in various applications.The FPeLEDs inherit the unique optical properties of metal halide perovskites,such as tunable bandgap,narrow emission linewidth,high photoluminescence quantum yield,and particularly,the soft nature of lattice.At present,substantial efforts have been made for FPeLEDs with encouraging external quantum efficiency(EQE)of 24.5%.Herein,we summarize the recent progress in FPeLEDs,focusing on the strategy developed for perovskite emission layers and flexible electrodes to facilitate the optoelectrical and mechanical performance.In addition,we present relevant applications of FPeLEDs in displays and beyond.Finally,perspective toward the future development and applications of flexible PeLEDs are also discussed.

Enhancing the Performance of Perovskite Light-Emitting Diodes via Synergistic Effect of Defect Passivation and Dielectric Screening

Metal halide perovskites,particularly the quasi-two-dimensional perovskite subclass,have exhibited considerable potential for next-generation electroluminescent materials for lighting and display.Nevertheless,the presence of defects within these perovskites has a substantial influence on the emission efficiency and durability of the devices.In this study,we revealed a synergistic passivation mechanism on perovskite films by using a dual-functional compound of potassium bromide.The dual functional potassium bromide on the one hand can passivate the defects of halide vacancies with bromine anions and,on the other hand,can screen the charged defects at the grain boundaries with potassium cations.This approach effectively reduces the probability of carriers quenching resulting from charged defects capture and consequently enhances the radiative recombination efficiency of perovskite thin films,leading to a significant enhancement of photoluminescence quantum yield to near-unity values(95%).Meanwhile,the potassium bromide treatment promoted the growth of homogeneous and smooth film,facilitating the charge carrier injection in the devices.Consequently,the perovskite light-emitting diodes based on this strategy achieve a maximum external quantum efficiency of~21%and maximum luminance of~60,000 cd m^(-2).This work provides a deeper insight into the passivation mechanism of ionic compound additives in perovskite with the solution method.

Recent Advances in Patterning Strategies for Full‑Color Perovskite Light‑Emitting Diodes

Metal halide perovskites have emerged as promising light-emitting materials for next-generation displays owing to their remarkable material characteristics including broad color tunability,pure color emission with remarkably narrow bandwidths,high quantum yield,and solution processability.Despite recent advances have pushed the luminance efficiency of monochromic perovskite light-emitting diodes(PeLEDs)to their theoretical limits,their current fabrication using the spincoating process poses limitations for fabrication of full-color displays.To integrate PeLEDs into full-color display panels,it is crucial to pattern red–green–blue(RGB)perovskite pixels,while mitigating issues such as cross-contamination and reductions in luminous efficiency.Herein,we present state-of-the-art patterning technologies for the development of full-color PeLEDs.First,we highlight recent advances in the development of efficient PeLEDs.Second,we discuss various patterning techniques of MPHs(i.e.,photolithography,inkjet printing,electron beam lithography and laserassisted lithography,electrohydrodynamic jet printing,thermal evaporation,and transfer printing)for fabrication of RGB pixelated displays.These patterning techniques can be classified into two distinct approaches:in situ crystallization patterning using perovskite precursors and patterning of colloidal perovskite nanocrystals.This review highlights advancements and limitations in patterning techniques for PeLEDs,paving the way for integrating PeLEDs into full-color panels.

Light-emitting diodes based on all-inorganic copper halide perovskite with self-trapped excitons

Light-emitting diodes based on lead halide perovskite have attracted great attention due to their outstanding performance.However,their application is plagued by the toxicity of Pb and the poor stability.Herein novel copper-based all inorganic perovskite CsCu2I3 with much enhanced stability has been reported with a potential photoluminescence quantum yield(PLQY)over 20%and self-trapped excitons(STE).By taking advantage of its extraordinary thermal stability,we successfully fabricate high-quality CsCu2I3 film through direct vacuum-based deposition(VBD)of CsCu2I3 powder.The resulting film shows almost the same PLQY with the synthesized powder,as well as excellent uniformity and stability.The perovskite light-emitting diodes(Pe-LED)based on the evaporated CsCu2I3 emitting layer achieve a luminescence of 10 cd/m2 and an external quantum efficiency(EQE)of 0.02%.To the best of our knowledge,this is the first CsCu2I3 Pe-LED fabricated by VBD with STE property,which offers a new avenue for lead-free Pe-LED.

The strategies for preparing blue perovskite light-emitting diodes

Metal halide perovskites have attracted tremendous interest due to their excellent optical and electrical properties,and they find many promising applications in the optoelectronic fields of solar cells,light-emitting diodes,and photodetectors.Thanks to the contributions of international researchers,significant progress has been made for perovskite light-emitting diodes(Pero-LEDs).The external quantum efficiencies(EQEs)of Pero-LEDs with emission of green,red,and near-infrared have all exceeded 20%.However,the blue Pero-LEDs still lag due to the poor film quality and deficient device structure.Herein,we summarize the strategies for preparing blue-emitting perovskites and categorize them into two:compositional engineering and size controlling of the emitting units.The advantages and disadvantages of both strategies are discussed,and a perspective of preparing high-performance blue-emitting perovskite is proposed.The challenges and future directions of blue PeroLEDs fabrication are also discussed.

Surface Treatment of Inorganic CsPbI_(3) Nanocrystals with Guanidinium Iodide for Efficient Perovskite Light-Emitting Diodes with High Brightness

The remarkable evolution of metal halide perovskites in the past decade makes them promise for next-generation optoelectronic material.In particular,nanocrystals(NCs)of inorganic perovskites have demonstrated excellent performance for light-emitting and display applications.However,the presence of surface defects on the NCs negatively impacts their performance in devices.Herein,we report a compatible facial post-treatment of CsPbI_(3) nanocrystals using guanidinium iodide(GuI).It is found that the GuI treatment effectively passivated the halide vacancy defects on the surface of the NCs while offering effective surface protection and exciton confinement thanks to the beneficial contribution of iodide and guanidinium cation.As a consequence,the film of treated CsPbI_(3) nanocrystals exhibited significantly enhanced luminescence and charge transport properties,leading to high-performance light-emitting diode with maximum external quantum efficiency of 13.8%with high brightness(peak luminance of 7039 cd m^(−2) and a peak current density of 10.8 cd A^(−1)).The EQE is over threefold higher than performance of untreated device(EQE:3.8%).The operational half-lifetime of the treated devices also was significantly improved with T50 of 20 min(at current density of 25 mA cm^(−2)),outperforming the untreated devices(T50~6 min).

Giant efficiency and color purity enhancement in multicolor inorganic perovskite light-emitting diodes via heating-assisted vacuum deposition

Inorganic perovskites(Cs Pb X3(X=I,Br,Cl))have broad prospection in the field of high-definition displaying due to its excellent optoelectronic characteristics.The vacuum deposition process possesses advantages and competitiveness in the industrialized production.However,the performance of light emitting diodes(LEDs)based on vacuum-deposited is incredibly low.Herein,we proposed a heating-assisted vacuum deposition(HAVD)method to construct inorganic perovskite LEDs(Pe LEDs)with enhanced performance.The roughness and crystallinity of perovskite film were improved by regulating the heating treatment of substrates.And the perovskite film exhibited largely rise in luminescence,with decreasing defect density.Consequently,with the optimized temperature,the green Pe LEDs exhibited 100-fold improvement of external quantum efficiency(EQE)with the luminance of up to 11941 cd/m2,and the full width at half-maximum(FWHM)of the electroluminescence(EL)spectra was decreased from 25 to 17 nm.At the same time,the red and blue Pe LEDs also exhibited obvious enhancement in EQE and luminance by HAVD method,and both the FWHM of EL spectra dropped below 20 nm,exhibiting excellent high color purity.HAVD strategy has a huge potential to be a new commonly used method for low-cost fabrication of displays and lighting.

Large-area fabrication:The next target of perovskite light-emitting diodes

Perovskite materials show exciting potential for light-emitting diodes(LEDs)owing to their intrinsically high photoluminescence efficiency and color purity.The research focusing on perovskite light-emitting diodes(PeLEDs)has experienced an exponential growth in the past six years.The maximum external quantum efficiency of red,green,and blue PeLEDs has surpassed 20%,20%,and 10%,respectively.Nevertheless,the current PeLEDs are still in the laboratory stage,and the key for further development of PeLEDs is large-area fabrication.In this paper,we briefly discuss the similarities and differences between manufacturing high-quality and large-area PeLEDs and perovskite solar cells.Especially,the general technologies for fabricating large-area perovskite films are also introduced.The effect of charge transport layers and electrodes on large-area devices are discussed as well.Most importantly,we summarize the advances of large-area(active area≥30 mm^(2))PeLEDs reported since 2017,and describe the methods for optimizing large-area PeLEDs reported in the literature.Finally,the development perspective of PeLEDs is presented for the goal of highly efficient and large-area PeLED fabrication.It is of great significance for the application of PeLEDs in future display and lighting.

Effect of different bending shapes on thermal properties of flexible light-emitting diode filament

Heat dissipation is an important part of light-emitting diode(LED)filament research and has aroused constant concern.In this paper,we studied the thermal performance of flexible LED filament by numerical simulation and through experiment.The heat dissipation characteristics of spring-like structure flexible LED filament were computed by finite volume method,and it was found that the chip junction temperature was closely related to the pitch and the bending radius.The effect of inclination angle of lighting LED filament was discussed because it is relevant to the spring-like structure flexible LED filament in geometry.The results demonstrated that the temperature of the filament increases as the inclination angle improves.

Proton‑Prompted Ligand Exchange to Achieve High‑Efficiency CsPbI_(3) Quantum Dot Light‑Emitting Diodes

CsPbI_(3)perovskite quantum dots(QDs)are ideal materials for the next generation of red light-emitting diodes.However,the low phase stability of CsPbI_(3)QDs and long-chain insulating capping ligands hinder the improvement of device performance.Traditional in-situ ligand replacement and ligand exchange after synthesis were often difficult to control.Here,we proposed a new ligand exchange strategy using a proton-prompted insitu exchange of short 5-aminopentanoic acid ligands with long-chain oleic acid and oleylamine ligands to obtain stable small-size CsPbI_(3)QDs.This exchange strategy maintained the size and morphology of CsPbI_(3)QDs and improved the optical properties and the conductivity of CsPbI_(3)QDs films.As a result,high-efficiency red QD-based light-emitting diodes with an emission wavelength of 645 nm demonstrated a record maximum external quantum efficiency of 24.45%and an operational half-life of 10.79 h.

Revealing the vertical structure of in-situ fabricated perovskite nanocrystals films toward efficient pure red light-emitting diodes

The development of efficient perovskite light-emitting diodes(PeLEDs)relies strongly on the fabrication of perovskite films with rationally designed structures(grain size,composition,surface,etc.).Therefore,an understanding of structure-performance relationships is of vital importance for developing high-performance perovskite devices,particularly for devices with in-situ fabricated perovskite nanocrystal films.In this study,we reveal the vertical structure of an in-situ fabricated quasi-two-dimensional perovskite film.By combining time-of-flight secondary ion mass spectrometry,energy dispersive spectroscopy,grazing incidence wide-angle X-ray scattering(GIWAXS),and low-temperature photoluminescence spectra,we illustrate that the resulting in-situ fabricated DPPA_(2)Cs_(n-1)Pb_(n)(Br_(0.3)I_(0.7))_(3n+1)(DPPA^(+):3,3-diphenylpropylammonium)film has a gradient structure with a very thin layer of ligands on the surface,predominantly small-n domains at the top,and predominantly large-n domains at the bottom owing to the solubility difference of the precursors.In addition,GIWAXS measurements show that the domain of n=2 on the top layer has an ordered in-plane alignment.Based on the understanding of the film structure,we developed an in-situ fabrication process with ligand exchange to achieve efficient pure red PeLEDs at 638 nm with an average external quantum efficiency(EQE)of 7.4%.The optimized device had a maximum luminance of 623 cd/m^(2) with a peak EQE of 9.7%.

Formadinium Cation Doping Stabilized Ultra-deep-blue Lead Halide Perovskite Nanocrystal Light-emitting Diodes

The halide migration effect in mixed-halide lead-based perovskite is a serious problem hindering the development of its display technology.In this study,we have successfully addressed this issue by reporting formadinium(FA)doped mixed-halide perovskite nanocrystals(NCs)with ultra-deep-blue emission of 450 nm,narrow bandwidth of 16 nm,and a high photoluminescence quantum yield(PLQY)of 66%.The perovskite nanocrystal light-emitting diodes(NC-LEDs)using this nanocrystal as an active layer achieved a maximum external quantum efficiency(EQE)of 0.32%,30-fold improved compared to that of pristine and stable electroluminescence(EL)spectra at 450 nm under a 4.9–8.0 V bias.These findings demonstrate the potential of our approach in developing stable and efficient deep blue perovskite NC-LEDs.

Self‑Generated Buried Submicrocavities for High‑Performance Near‑Infrared Perovskite Light‑Emitting Diode

ABSTRACT Embedding submicrocavities is an effective approach to improve the light out-coupling efficiency(LOCE)for planar perovskite light-emitting diodes(PeLEDs).In this work,we employ phenethylammonium iodide(PEAI)to trigger the Ostwald ripening for the downward recrystallization of perovskite,resulting in spontaneous formation of buried submicrocavities as light output coupler.The simulation suggests the buried submicrocavities can improve the LOCE from 26.8 to 36.2%for near-infrared light.Therefore,PeLED yields peak external quantum efficiency(EQE)increasing from 17.3%at current density of 114 mA cm^(−2)to 25.5%at current density of 109 mA cm^(−2)and a radiance increasing from 109 to 487 W sr^(−1)m^(−2)with low rolling-off.The turn-on voltage decreased from 1.25 to 1.15 V at 0.1 W sr^(−1)m^(−2).Besides,downward recrystallization process slightly reduces the trap density from 8.90×10^(15)to 7.27×10^(15)cm^(−3).This work provides a self-assembly method to integrate buried output coupler for boosting the performance of PeLEDs.

Advances and Challenges in Two‑Dimensional Organic–Inorganic Hybrid Perovskites Toward High‑Performance Light‑Emitting Diodes

Two-dimensional(2D)perovskites are known as one of the most promising luminescent materials due to their structural diversity and outstanding optoelectronic properties.Compared with 3D perovskites,2D perovskites have natural quantum well structures,large exciton binding energy(Eb)and outstanding thermal stability,which shows great potential in the next-generation displays and solidstate lighting.In this review,the fundamental structure,photophysical and electrical properties of 2D perovskite films were illustrated systematically.Based on the advantages of 2D perovskites,such as special energy funnel process,ultrafast energy transfer,dense film and low efficiency roll-off,the remarkable achievements of 2D perovskite light-emitting diodes(PeLEDs)are summarized,and exciting challenges of 2D perovskite are also discussed.An outlook on further improving the efficiency of pure-blue PeLEDs,enhancing the operational stability of PeLEDs and reducing the toxicity to push this field forward was also provided.This review provides an overview of the recent developments of 2D perovskite materials and LED applications,and outlining challenges for achieving the high-performance devices.

Developments and challenges ahead in blue perovskite light-emitting devices

Recently,perovskite light-emitting diodes(Pe LEDs)have developed rapidly in the green,red,and nearinfrared light emissions,owing to the unique optoelectronic characteristics of halide perovskites,such as high carrier mobility,narrow emission linewidths,high photoluminescence quantum yield,as well as bandgap tunability.However,the efficiency improvement in blue(especially deep-blue)Pe LEDs is still inferior to other analogs,which severely restricts the Pe LED applications.Here,we systematically summarize the substantial progress in the performance of blue Pe LEDs based on different blue perovskite candidates,and recent advances from three aspects(i.e.,the sky-blue,pure-blue,and deep-blue light emissions).Then,we point out several challenges existing in deep-blue Pe LEDs,such as the effect of Cl-ions incorporation,spectral instability,ion migration,and the difficulty of charge injection,and highlight the strategies to improve device efficiency,to motivate further research and development of blue Pe LEDs.

980 nm Near-Infrared Light-Emitting Diode Using All-Inorganic Perovskite Nanocrystals Doped with Ytterbium Ions

All-inorganic perovskite(CsPbX3)nanocrystals(NCs)have recently been widely investigated as versatile solution-processable light-emitting materials.Due to its wide-bandgap nature,the all-inorganic perovskite NC Light-Emitting Diode(LED)is limited to the visible region(400-700 nm).A particularly difficult challenge lies in the practical application of perovskite NCs in the infrared-spectrum region.In this work,a 980 nm NIR all-inorganic perovskite NC LED is demonstrated,which is based on an efficient energy transfer from wide-bandgap materials(CsPbCl3 NCs)to ytterbium ions(Yb3+)as an NIR emitter doped in perovskite NCs.The optimized CsPbCl3 NC with 15 mol%Yb3+doping concentration has the strongest 980 nm photoluminescence(PL)peak,with a PL quantum yield of 63%.An inverted perovskite NC LED is fabricated with the structure of ITO/PEDOT:PSS/poly-TPD/CsPbCl3:15 mol%Yb3+NCs/TPBi/LiF/Al.The LED has an External Quantum Efficiency(EQE)of 0.2%,a Full Width at Half Maximum(FWHM)of 47 nm,and a maximum luminescence of 182 cd/m?.The introduction of Yb3+doping in perovskite NCs makes it possible to expand its working wavelength to near-infrared band for next-generation light sources and shows potential applications for optoelectronic integration.

Rapid crystallization-driven high-efficiency phase-pure deep-blue Ruddlesden–Popper perovskite light-emitting diodes

Perovskite light-emitting diodes(PeLEDs)are considered as promising candidates for nextgeneration solution-processed full-color displays.However,the external quantum efficiencies(EQEs)and operational stabilities of deep-blue(<460 nm)PeLEDs still lag far behind their red and green counterparts.Herein,a rapid crystallization method based on hot-antisolvent bathing is proposed for realization of deep-blue PeLEDs.By promoting immediate removal of the precursor solvent from the wet perovskite films,development of the quasi-two-dimensional(2D)Ruddlesden–Popper perovskite(2D-RPP)crystals with n values>3 is hampered completely,so that phase-pure 2D-RPP films with bandgaps suitable for deep-blue PeLEDs can be obtained successfully.The uniquely developed rapid crystallization method also enables formation of randomly oriented 2D-RPP crystals,thereby improving the transfer and transport kinetics of the charge carriers.Thus,high-performance deep-blue PeLEDs emitting at 437 nm with a peak EQE of 0.63%are successfully demonstrated.The color coordinates are confirmed to be(0.165,0.044),which match well with the Rec.2020 standard blue gamut and have excellent spectral stability.

Perovskite light-emitting diodes toward commercial full-colour displays:progress and key technical obstacles

Metal-halide perovskite light-emitting diodes(PeLEDs)possess wide colour gamut,high luminescence efficiency,and low-cost synthesis,making them a promising photonic source for next-generation display applications.Since the first room-temperature emission PeLED was demonstrated in 2014,their performance has improved rapidly within a few years,leading to considerable attention from academia and industry.In this review,we discuss the primary technical bottlenecks of PeLEDs for commercial display applications,including large-area PeLED preparation,patterning strategies,and flexible PeLED devices.We review the technical approaches for achieving these targets and highlight the current challenges while providing an outlook for these perovskite materials and PeLED devices to meet the requirements of the next-generation high-colour-purity full-colour display market.

Heterointerface engineering of perovskite defects and energetics for light-emitting diodes

Perovskite light-emitting diodes(PeLEDs)rely on optimized device architecture to realize effective electro-optical converting.Especially,the stacks of dissimilar semiconducting materials form heterointerfaces,at which the defects and energetics of perovskite film greatly affect the device performance.Herein,we focus on the heterointerface engineering of perovskite towards high-quality PeLEDs.The defect engineering at both the bottom-surface(namely buried interface)and top-surface of perovskite film is simultaneously performed by semiconducting passivating molecules,which feature aligned energy levels and superior carrier injection ability regarding to perovskite.Moreover,such defect passivation could influence the heterointerface energetics.The perovskite work function is decreased by our suggested passivator treatment because of interface dipole,which results in band bending at the heterojunction and modulates the carrier dynamics.Hence,the electron injection is greatly enhanced,which boosts the up-conversion electroluminescence in current system.Overall,via the heterointerface engineering of defects and energetics synergistically,efficient PeLEDs with 3-fold enhancement of external quantum efficiency and low driving voltages with respect to pristine ones are achieved based on our proposed PeLED architecture.

Stably doped graphene transparent electrode with improved lightextraction for efficient flexible organic light-emitting diodes

Graphene-based flexible transparent electrodes(FTEs)are promising candidate materials for developing next-generation flexible organic light-emitting diodes(OLEDs).However,the quest for high-efficiency OLEDs is hindered by the low light-extraction and charge injection efficiencies of graphene electrode.Here,we combine the frustrated Lewis pair doping with nanostructure engineering to obtain high-performance graphene FTE.A p-type dopant aci-nitromethane-tris(pentafluorophenyl)borane(ANBCF)was synthesized and deposited on graphene FTE to form an aperiodic nanostructure,which not only improves the light-extraction but also stably p-dopes graphene to enhance its hole injection.The use of ANBCF-doped graphene as the anode enables high-efficiency flexible green OLEDs with external quantum efficiency(EQE)and power efficiency(PE)out-performing most flexible graphene OLEDs of comparable structure.This study provides a simple and effective pathway to fabricate high-performance graphene FTEs for efficient flexible OLEDs.