Pure Blue Electroluminescence by Differentiated Ion Motion in a Single Layer Perovskite Device

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, CsPbBr_3−xCl_x perovskites, 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 CsPbBr₃ tunes 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 LiPF₆ inclusion 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.     

Strategies Toward Efficient Blue Perovskite Light-Emitting Diodes

Substantial progress has been made in blue perovskite light-emitting diodes (PeLEDs). In this review, the strategies for high-performance blue PeLEDs are described, and the main focus is on the optimization of the optical and electrical properties of perovskites. In detail, the fundamental device working principles are first elucidated, followed by a systematical discussion of the key issues for achieving high-quality perovskite nanocrystals (NCs) and quasi-2D perovskites. These involve ligand optimization and metal doping in enhancing the carrier transport and reducing the traps of perovskite NCs, as well as the perovskite phase modulation and defect passivation in improving energy transfer and emission efficiency of quasi-2D perovskites. The strategies for efficient 3D mixed-halide perovskite and lead-free perovskite blue LEDs are then briefly introduced. After that, other strategies, including effective charge transport layer, efficient perovskite emission system, and effective device architecture for high light outcoupling efficiency, are further discussed to boost the blue PeLED performances. Meanwhile, the testing standard of blue PeLED lifetime is suggested to enable the direct comparisons of the device operational stability. Finally, challenges and future directions for blue PeLEDs are addressed.     

Synergistic Effect of Dual Ligands on Stable Blue Quasi‐2D Perovskite Light‐Emitting Diodes

Since the emergence of inorganic–organic hybrid perovskites a few years ago, there have been many promising achievements in the field of green and red perovskite light‐emitting diodes (PeLEDs). Nevertheless, the performance of blue‐light PeLEDs faces challenges. In this work, the unique synergy obtained by introducing two different ligands to successfully form quasi‐2D perovskite films, which can exhibit stable blue‐light emission, is utilized. The fabricated PeLEDs have a maximum external quantum efficiency of 2.62% and a half lifetime (T₅₀) of 8.8 min. Meanwhile, the electroluminescence spectrum with its peak located at 485 nm, demonstrates improved stability by applying different voltage bias. The finding in this work offers a new way to achieve steady blue PeLEDs with high performance.     

Interfacial Nucleation Seeding for Electroluminescent Manipulation in Blue Perovskite Light-Emitting Diodes

Efficient and stable blue emission of perovskite light-emitting diodes (PeLEDs) is a requisite toward their potential applications in full-color displays and solid-state lighting. Rational manipulation over the entire electroluminescence process is promising to break the efficiency limit of blue PeLEDs. Herein, a facile device architecture is proposed to achieve efficient blue PeLEDs for simultaneously reducing the energetic loss during electron-photon conversion and boosting the light outcoupling. Effective interfacial engineering is employed to manipulate the perovskite crystallization nucleation, enabling highly compact perovskite nanocrystal assemblies and suppressing the trap-induced carrier losses by means of interfacial hydrogen bonding interactions. This strategy contributes to a high external quantum efficiency (EQE) of 12.8% for blue PeLEDs emitting at 486 nm as well as improved operational stability. Moreover, blue PeLEDs reach a peak EQE of 16.8% with the incorporation of internal outcoupling structures for waveguided light, which can be further raised to 27.5% by integrating a lens-based structure for substrate-mode light. These results verify the validity of this strategy in producing efficient and stable blue PeLEDs for practical applications.     

High-Performance Blue Perovskite Films and Micro-Arrays for Light-Emitting Diodes with Ionic Liquid Interlayer

Metal halide perovskites have attracted considerable attention for light-emitting diode (LED) applications due to their desirable optoelectronic properties including high brightness and color purity. However, the performance of blue perovskite LEDs (PeLEDs) remains inferior to their red and green counterparts. Herein, an ionic liquid (IL), specifically 1-butyl-3-methylimidazolium tetrafluoroborate is introduced as the interlayer on the hole transport layer (HTL). This IL demonstrates a strong interaction with the perovskite emissive layer, resulting in effective defect passivation and a shallower valence band maximum. Consequently, nonradiative recombination is reduced, and hole injection is enhanced. Additionally, a soft lithography method employing a transfer process is successfully developed that enables precise micropatterning of the perovskite light-emitting layer. Through these advancements, the IL-modified PeLED exhibits pure blue emission at 470 nm with a maximum luminance of 891 cd m⁻² and an impressive maximum EQE of 8.3%. Furthermore, the micro PeLED with an IL interlayer achieves a maximum luminance of 400 cd m⁻² and a maximum EQE of 3.9%.     

Tetraphenylimidazole‐Based Excited‐State Intramolecular Proton‐Transfer Molecules for Highly Efficient Blue Electroluminescence

Aiming for highly efficient blue electroluminescence, we have designed and synthesized a novel class of tetraphenylimidazole‐ based excited‐state intramolecular proton‐transfer (ESIPT) molecules with covalently linked charge‐transporting functional groups (carbazole‐ and oxadiazole‐functionalized hydroxyl‐substituted tetraphenylimidazole (HPI), i.e., HPI‐Cbz and HPI‐Oxd, respectively). High T_g (ca. 130 °C) amorphous films of HPI‐Cbz and HPI‐Oxd showed intense and ideal blue‐light emission (λ_max = 462 and 468 nm, Φ_PL = 0.44 and 0.38) with a large Stokes shift of over 160 nm and a narrow full width at half‐maximum of less than 65 nm. Organic light‐emitting devices using HPI‐Cbz and HPI‐Oxd as the emitting layer generated an efficient blue electroluminescence (EL) emission peaking at around 460 nm with excellent CIE coordinates of (x, y) = (0.15, 0.11). A maximum external quantum efficiency of 2.94%, and a maximum brightness of 1 229 cd m⁻² at 100 mA cm⁻², as well as a low turn‐on voltage of 4.8 V were achieved in this work.     

Polymer-Encapsulated Halide Perovskite Color Converters to Overcome Blue Overshoot and Cyan Gap of White Light-Emitting Diodes

Currently, the most popular way to manufacture white light-emitting diodes (WLEDs) is based on blue-emitting InGaN LED chips (440–460 nm) and yellow-emitting phosphor coating (520–700 nm) to produce white light lighting. However, because conventional white WLEDs lack the uniformly distributed continuous emission spectrum compared to natural sunlight: “blue overshoot” (extra 440–460 nm blue-light can cause damage to the retina) and “cyan gap” (470–520 nm wavelength range). Here, a novel strategy to “kill two birds with one stone” is reported: using the stable and bright polymer encapsulated perovskite nanocrystals (PNCs) composite films as the cyan color converters that efficiently absorb the “blue overshoot” and effectively emit the cyan light to fill the “cyan gap”. A series of polymer-encapsulated PNC films is achieved that can reach very high photoluminescence quantum yield (PL QY) of 90–95% under 450 nm blue-light excitation. Importantly, both 370 nm UV-excited WLED and 455 nm blue-excited WLED devices are constructed that exhibit smoothly and evenly distributed white light without blue overshoot and cyan gap, which was not achieved before for blue-excited cyan-emissive materials. This study paves the way toward the application of PNC color converters in the next generation full-visible-spectrum WLED lighting that mimic the natural daylight.     

Highly Efficient 1D/3D Ferroelectric Perovskite Solar Cell

With the capability to manipulate the built-in field in solar cells, ferroelectricity is found to be a promising attribute for harvesting solar energy in solar cell devices by influencing associated device parameters. Researchers have devoted themselves to the exploration of ferroelectric materials that simultaneously possess strong light absorption and good electric transport properties for a long time. Here, it is presented a novel and facile approach of combining state-of-art light absorption and electric transport properties with ferroelectricity by the incorporation of room temperature 1D ferroelectric perovskite with 3D organic–inorganic hybrid perovskite (OIHP). The 1D/3D mixed OIHP films are found to exhibit evident ferroelectric properties. It is notable that the poling of the 1D/3D mixed ferroelectric OIHP solar cell can increase the average V_oc can be increased from 1.13 to 1.16 V, the average PCE from 20.7% to 21.5%. A maximum power conversion efficiency of 22.7%, along with an enhanced fill factor of over 80% and open-circuit voltage of 1.19 V, can be achieved in the champion device. The enhancement is by virtue of reduced surface recombination by ferroelectricity-induced modification of the built-in field. The maximum power point tracking measurement substantiates the retention of ferroelectric-polarization during the continued operation.     

Domain Controlling by Compound Additive toward Highly Efficient Quasi-2D Perovskite Light-Emitting Diodes

Quasi-2D perovskites with enlarged exciton binding energy and tunable bandgap are appealing for application in perovskite light-emitting diodes (PeLEDs). However, wide n domains distribution is commonly formed in solution-processed quasi-2D perovskite films due to the uncontrollable crystallization behavior, which leads to low device performance. Here, the crystallization process is successfully regulated to narrow the n domains distribution by introducing compound additive of ZrO₂ nanoparticles (NPs) and Cryptand complexant. ZrO₂ NPs can avoid the segregation of organic large and small cations by strengthening the solvent extraction capacity of antisolvent, while Cryptand offsets the poor solubility of PbBr₂ by forming an intermediate state to slow down the crystallization of high-n domains. Consequently, both high photoluminescence quantum yields over 90% and a high external quantum efficiency of 21.2% are obtained in the optimized green quasi-2D PeLEDs. Moreover, the lifetime extends about four times compared with control devices. The strategy of domain controlling by compound additive provides a powerful way to develop high-performance quasi-2D perovskite optoelectrical devices.     

Holy Water: Photo-Brightening in Quasi-2D Perovskite Films under Ambient Enables Highly Performing Light-Emitting Diodes

Quasi-2D perovskites provide new opportunities for lighting and display applications due to their high radiative recombination and excellent stability. However, seldom attention has been placed on their self-stability/working operation under ambient storage. Herein, quasi-2D perovskites/Polyethylene oxide (PEO) films are studied, showing an unforeseen photo-brightening effect under ambient storage (i.e., an increase of the photoluminescence quantum yield from 55% to 74% after 100 days). In stark contrast, those stored under a dark/inert atmosphere show a significant decrease down to 38%. This counterintuitive phenomenon responds to the increasing radiative recombination rate caused by the passivation of the surface Br vacancies in the presence of physically adsorbed water molecules, as corroborated by in situ/ex situ X-ray photoelectron spectroscopy and density functional theory calculations. Capitalizing on this surprising effect, stable light-emitting diodes (LEDs) using quasi-2D perovskites/PEO color filters are fabricated, realizing high stabilities of ≈400 h@10 mA under operating ambient conditions, representing a 20-fold enhancement compared to LEDs with 3D counter partners. Hence, this study reveals a unique insight into the impact of water passivation on the optical/structural properties of quasi-2D perovskite films, broadening their applications under operating ambient conditions.     

2D Ruddlesden–Popper Perovskite Nanoplate Based Deep‐Blue Light‐Emitting Diodes for Light Communication

Ruddlesden–Popper perovskite, (PEA)₂PbBr₄ (PEA = C₈H₉NH₃), is a steady and inexpensive material with a broad bandgap and a narrow‐band emission. These features make it a potential candidate for deep‐blue light‐emitting diodes (LEDs). However, due to the weak exciton binding energy, LEDs based on the perovskite thin films usually possess a very low external quantum efficiency (EQE) of <0.03%. Here, for the first time, the construction of high‐performance deep‐blue LEDs based on 2D (PEA)₂PbBr₄ nanoplates (NPs) is demonstrated. The as‐fabricated (PEA)₂PbBr₄ NPs film shows a deep‐blue emission at 410 nm with excellent stability under ambient conditions. Impressively, LEDs based on the (PEA)₂PbBr₄ NPs film deliver a bright deep‐blue emission with a maximum luminance of 147.6 cd m^?2 and a high EQE up to 0.31%, which represents the most efficient and brightest perovskite LEDs operating at deep‐blue wavelengths. Furthermore, the LEDs retain over 80% of their efficiencies for over 1350 min under ≈60% relative humidity. The steady and bright deep‐blue LEDs can be used as an excitation light source to realize white light emission, which shows the potential for light communication. The work provides scope for developing perovskite into efficient and deep‐blue LEDs for low‐cost light source and light communication.     

Hole Transport Bilayer Structure for Quasi‐2D Perovskite Based Blue Light‐Emitting Diodes with High Brightness and Good Spectral Stability

Substantial achievements have been made in green and red perovskite light emitting diodes (PeLEDs) recently. However, blue PeLEDs still lag behind with much lower performances. One of the main reasons is the mass undesirable nonradiative recombination at interfaces and within the perovskite films. In this work, an efficient hole transport bi‐layer structure composed of PSSNa and NiO_x is demonstrated to simultaneously inhibit the nonradiative decays between NiO_x and perovskite films by reducing NiO_x surface defects and improving quasi‐2D perovskite thin film quality by minimizing its pin‐holes and reducing the film roughness. The results show that the dipole feature of PSSNa improves the hole transportation and thus PeLED performances. Moreover, by introducing KBr into the perovskite, its film quality improves and trap states reduce. Eventually, the blue PeLEDs is achieved with a very low turn‐on voltage of 3.31 V accompanied with an external quantum efficiency of 1.45% and a remarkable luminance of 4359 cd m^‐2. With further optimization of the perovskite precursor concentration, the highest luminance reaches 5737 cd m^‐2, which represents the brightest blue PeLEDs reported to date as far as it is known. Furthermore, the devices also show better spectral stability and operation lifetime as compared to other blue PeLEDs.     

Efficient Blue Perovskite Light‐Emitting Diodes Boosted by 2D/3D Energy Cascade Channels

Lead halide perovskite, as an emerging semiconductor, provides a fire‐new opportunity for high‐definition display and solid‐state lighting. Earthshaking improvements are implemented in green, red, and near‐infrared perovskite light‐emitting diodes (PeLEDs). However, blue PeLEDs are still far behind in performance, which restricts the development of PeLEDs in practical applications. Herein, a facile energy cascade channel strategy via one‐step self‐organized and controllable 2D/3D perovskite preparation by introducing guanidine hydrobromide (GABr) is developed that greatly improves the efficiency of blue PeLEDs. The 2D/3D perovskite structure boosts the energy cascade to induce energy transfer from the wide into the narrow bandgap domains and inhibit free charge diffusion, which increases the density of electrons and holes, and enhances the radiative recombination. Profiting from this energy cascade channels, the external quantum efficiency of blue PeLEDs, emitting at 492 nm, is considerably enhanced from 1.5% of initial blue device to 8.2%. In addition, device operating stability under ambient conditions is also improved by 2.6‐fold. The one‐step self‐organized 2D/3D hybrid perovskites induced by GABr pave a new and simple route toward high‐performance blue emission PeLEDs.     

In Situ Growth of 2D Perovskite Capping Layer for Stable and Efficient Perovskite Solar Cells

2D halide perovskites have recently been recognized as a promising avenue in perovskite solar cells (PSCs) in terms of encouraging stability and defect passivation effect. However, the efficiency (less than 15%) of ultrastable 2D Ruddlesden–Popper PSCs still lag far behind their traditional 3D perovskite counterparts. Here, a rationally designed 2D‐3D perovskite stacking‐layered architecture by in situ growing 2D PEA₂PbI₄ capping layers on top of 3D perovskite film, which drastically improves the stability of PSCs without compromising their high performance, is reported. Such a 2D perovskite capping layer induces larger Fermi‐level splitting in the 2D‐3D perovskite film under light illumination, resulting in an enhanced open‐circuit voltage (V_oc) and thus a higher efficiency of 18.51% in the 2D‐3D PSCs. Time‐resolved photoluminescence decay measurements indicate the facilitated hole extraction in the 2D‐3D stacking‐layered perovskite films, which is ascribed to the optimized energy band alignment and reduced nonradiative recombination at the subgap states. Benefiting from the high moisture resistivity as well as suppressed ion migration of the 2D perovskite, the 2D‐3D PSCs show significantly improved long‐term stability, retaining nearly 90% of the initial power conversion efficiency after 1000 h exposure in the ambient conditions with a high relative humidity level of 60 ± 10%.     

Highly Efficient Blue Light-Emitting Diodes Based on Perovskite Film with Vertically Graded Bandgap and Organic Grain Boundary Passivation Shells

Metal halide perovskite materials have emerged as a promising class of semiconductors for high-performance optoelectronic applications, particularly for light-emitting diodes (LEDs), due to their high quantum efficiency, facile color tunability, narrow emission line widths, as well as cost-effectiveness. Despite the great successes on green and red perovskite LEDs (PeLEDs), the external quantum efficiency (EQE) of blue PeLEDs still lags far behind that of green and red counterparts. Here, wavelength tunable pure and deep blue PeLEDs with high EQE are presented, achieving 17.5% and 10.8% for emission wavelengths of 472 and 461 nm, respectively. The wavelength tenability and high EQE are attributed to the unique vertically graded bandgaps and grain boundary organic shells in the perovskite films. The results demonstrate a significant performance improvement in blue PeLEDs, provide a novel route to fabricate high-performance pure and deep blue PeLEDs that can match the performance of the green and red PeLEDs for future lighting and display applications.     

光致激励的有机薄膜器件的电致发光特性

为了研究有机电致发光器件(OLED)在高亮度下存在的电流下降现象,在不同强度的荧光激发下观察了单层和双层器件的电流密度(J-V)特性和电致(EL)光谱。在单层器件中发现,随着激发光的增强,发生了电流密度下降以及光谱蓝移现象,这是因为在低迁移率的有机物中,过剩的阴离子基对光子的强烈吸收,从而导致了载流子浓度的降低。在单层器件中插入4个不同厚度的空穴传输材料组成双层器件以平衡过剩的阴离子基,结果发现,随着厚度的增加电流密度下降和光谱蓝移的程度减少,当厚度超过50nm后,这种减少的程度变化不大。研究表明,插入适当厚度的空穴传输层能够抑制器件中的电流下降现象。     

Band Edge Control of Quasi-2D Metal Halide Perovskites for Blue Light-Emitting Diodes with Enhanced Performance

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.     

Quasi‐2D Inorganic CsPbBr3 Perovskite for Efficient and Stable Light‐Emitting Diodes

Metal halide perovskites are rising as a competitive material for next‐generation light‐emitting diodes (LEDs). However, the development of perovskite LEDs is impeded by their fast carriers diffusion and poor stability in bias condition. Herein, quasi‐2D CsPbBr₃ quantum wells homogeneously surrounded by inorganic crystalline Cs₄PbBr₆ of large bandgap are grown. The centralization of carriers in nanoregion facilitates radiative recombination and brings much enhanced luminescence quantum yield. The external quantum efficiency and luminescence intensity of the LEDs based on this nanocomposite are one order of magnitude higher than the conventional low‐dimensional perovskite. Meanwhile, the use of inorganic nanocomposite materials brings much improved device operation lifetime under constant electrical field.     

调整空穴传输层厚度改善蓝光有机器件的性能

利用有机发光材料N，N’-bis-（1-naphthyt）N，N’-diphenyl-1，1’-biphenyl-4，4＇-diamine（NPB）作为空穴传输层。4,4-dis（2，2’diphenytvinyl）-1，1’-biphenyl（DPVBi）作为发光层，aluminium-tris-8-hydroxy—quinoline（Alq3）作为电子传输层。采用ITO／NPB／DPVBi／Alq3／LiF／Al基本结构，研究了NPB厚度对蓝光有机器件（OLED）的亮度和效率的影响。在DPVBi、Alq3、LiF和Al分别保持在20、30、0．5和100nm不变。而NPB在40、50…和150nm内进行变化，在NPB小于130nm而大于40nm内，亮度随厚度的增加而增加，最大亮度达到6891cd／m^2，对应的效率是1．64cd／A，而色（CIE）坐标的变化范围较小，获得了性能较好的蓝光OLED。     

High Efficiency and High Open Circuit Voltage in Quasi 2D Perovskite Based Solar Cells

An important property of hybrid layered perovskite is the possibility to reduce its dimensionality to provide wider band gap and better stability. In this work, 2D perovskite of the structure (PEA)₂(MA)_n–1Pb_nBr_3n+1 has been sensitized, where PEA is phenyl ethyl‐ammonium, MA is methyl‐ammonium, and using only bromide as the halide. The number of the perovskite layers has been varied (n) from n = 1 through n = ∞. Optical and physical characterization verify the layered structure and the increase in the band gap. The photovoltaic performance shows higher open circuit voltage (V_oc) for the quasi 2D perovskite (i.e., n = 40, 50, 60) compared to the 3D perovskite. V_oc of 1.3 V without hole transport material (HTM) and V_oc of 1.46 V using HTM have been demonstrated, with corresponding efficiency of 6.3% and 8.5%, among the highest reported. The lower mobility and transport in the quasi 2D perovskites have been proved effective to gain high V_oc with high efficiency, further supported by ab initio calculations and charge extraction measurements. Bromide is the only halide used in these quasi 2D perovskites, as mixing halides have recently revealed instability of the perovskite structure. These quasi 2D materials are promising candidates for use in optoelectronic applications that simultaneously require high voltage and high efficiency.