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1.
    
Perovskite light-emitting diodes (PeLEDs) have garnered extraordinary attention in displaying field owing to their excellent luminescence properties. Although exogenous additives are extensively employed for optimizing PeLEDs, their comprehensive regulation including side effects still lacks in-depth study. Here for the first time, it is demonstrated that the deprotonation degree of additives significantly influences the performance of blue PeLEDs. Benzenesulfonic acid (BSA) and ammonium benzenesulfonate (ABS) with similar molecular structures while distinctly different acid dissociation constants (pKa) are used for modifying blue perovskites. By comparison, high-pKa ABS holds greater potential in boosting device performance, contributing to an improved peak external quantum efficiency of 18.8%. This discrepancy is ascribed to the fact that low-pKa BSA is prone to induce prominent perovskite chlorine loss owing to its intense deprotonation, while high-pKa ABS significantly suppresses chlorine vacancy formation. Meanwhile, the adsorption energy of organic spacer onto perovskite is greatly reduced due to the strong intermolecular hydrogen bonding with ABS, contributing to a concentrated phase arrangement for smooth exciton energy transfer. Additionally, ABS modification further suppresses trap-mediated nonradiative recombination by coordinating with the undercoordinated lead (II) ions at grain boundaries. This work provides valuable guidelines for optimizing additive screening toward high-performance blue PeLEDs.  相似文献   

2.
    
Hybrid organometal halide perovskites are known for their excellent optoelectronic functionality as well as their wide‐ranging chemical flexibility. The composition of hybrid perovskite devices has trended toward increasing complexity as fine‐tuned properties are pursued, including multielement mixing on the constituents A and B and halide sites. However, this tunability presents potential challenges for charge extraction in functional devices. Poor consistency and repeatability between devices may arise due to variations in composition and microstructure. Within a single device, spatial heterogeneity in composition and phase segregation may limit the device from achieving its performance potential. This review details how the nanoscale elemental distribution and charge collection in hybrid perovskite materials evolve as chemical complexity increases, highlighting recent results using nondestructive operando synchrotron‐based X‐ray nanoprobe techniques. The results reveal a strong link between local chemistry and charge collection that must be controlled to develop robust, high‐performance hybrid perovskite materials for optoelectronic devices.  相似文献   

3.
The two-step sequentially deposition strategy has been widely used to produce high-performance FAPbI3-based solar cells. However, due to the rapid reaction between PbI2 and FAI, a dense perovskite film forms on top of the PbI2 layer immediately and blocks the FAI diffusion into the bottom of the PbI2 film for a complete reaction, which results in a low-efficiency and limited reproducibility of perovskite solar cells (PSCs). Here, high-quality α-FAPbI3 perovskite films by crystal growth regulation with 4-fluorobenzamide additives is fabricated. The additives can interact with FAI to suppress the fast reaction between the FAI and PbI2 and effectively passivate the under-coordinated Pb2+ or I- defects. As a result, α-FAPbI3 perovskite films with low trap density and large grain size are prepared. The modified PSCs present a high-power conversion efficiency of 24.08%, maintaining 90% of their initial efficiency after 1400 h in high humidity. This study provides an efficient strategy of synergistic crystallization and passivation to form high-quality α-FAPbI3 films for high-performance PSCs.  相似文献   

4.
    
Metal halide perovskites have attracted a considerable amount of research attention with significant progress made in the field of optoelectronics. Despite their outstanding electrical characteristics, structural defects impede their potential performance due to the polycrystalline nature of solution-processed perovskite films. Herein, the effective p-type doping and defect passivation of phenethylammonium tin iodide ((PEA)2SnI4) perovskite films using xanthate additives as a sulfur source is reported. Sulfur can be introduced to the iodine vacancies mainly at the grain boundaries of the perovskite film, passivating the electrical defects originating from the iodine vacancy and increasing the hole concentration. The Fermi-level shift toward the valence band maximum of the sulfur-doped perovskite film is confirmed using ultraviolet photoemission spectroscopy, resulting in p-type doping. Finally, the electrical performance improvement for the 0.2% sulfur-doped (PEA)2SnI4 thin-film transistor with a mobility of 1.45 cm2 V−1 s−1, an on/off ratio of 2.9 × 105 is demonstrated, and hysteresis of 10 V is reduced.  相似文献   

5.
利用扫描电镜、能谱分析、光学轮廓仪以及金相显微镜等测试手段对液相外延碲镉汞薄膜表面缺陷的形貌、成分和断面进行了分析,并研究了不同种类表面缺陷的特征及来源。结果表明,液相外延碲镉汞薄膜表面上存在的结晶类缺陷往往尺寸较大或成片分布,对后续器件产生明显影响。通过分析其成因可以发现,母液均匀性的提升是减少该类缺陷和提高碲镉汞薄膜质量的关键。  相似文献   

6.
    
Multiple‐cation lead mixed‐halide perovskites (MLMPs) have been recognized as ideal candidates in perovskite solar cells in terms of high efficiency and stability due to decreased open‐circuit voltage loss and suppressed yellow phase formation. However, they still suffer from an unsatisfactory long‐term moisture stability. In this study, phosphorus‐containing Lewis acid and base molecules are employed to improve device efficiency and stability based on their multifunction including recombination reduction, phase segregation suppression, and moisture resistance. The strong fluorine‐containing Lewis acid treatment can achieve a champion PCE of 22.02%. Unencapsulated and encapsulated devices retain 63% and 80% of the initial efficiency after 14 days of aging under 75% and 85% relative humidity, respectively. The better passivation of Lewis acid implies more halide defects than Pb defects at the MLMP surface. This unbalanced defect type results from phase segregation that is the synergistic effect of Cs and halide ion migrations. Identifying defect type based on different passivation effects is beneficial to not only choose suitable passivators to boost the efficiency and slow down the moisture degradation of MLMP solar cells, but also to understand the mechanism of defect‐assisted moisture degradation.  相似文献   

7.
    
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.  相似文献   

8.
    
2D perovskites are widely employed to improve efficiency and stability of perovskite solar cells (PSCs), but the processes are rarely accomplished in air due to the difficulty of controlling the formation processes. An ultra-thin 2D capping layer with an alternating cation interlayer (ACI) structure is in situ formed by fumigating 3D perovskites with benzylamine vapor. The whole process is finished in air within 10 s regardless of the humidity, after which both defects and tensile strain are reduced and the interfacial energy band gets benignly aligned to a type-I heterojunction, avoiding direct charge recombination at the interface. Theoretical analysis reveals that the ACI phase is thermodynamically more stable than an analogous Ruddlesden–Popper phase. The strategy can passivate various perovskites, including methylammonium (or multi-cation) lead (or lead/tin mixed) halide perovskites, prepared via either vapor or solution approaches, increasing the absolute power conversion efficiency by up to 2.5%. It can uniformly passivate PSCs without area limitation, and provide a repeatable methodology for passivating perovskites.  相似文献   

9.
    
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%.  相似文献   

10.
研究了蓝相Ⅱ态液晶的双螺旋结构及特点,分析了缺陷与双螺旋结构的关系,解释了产生缺陷位置的原因。介绍了传统制作蓝相Ⅱ态液晶晶格模型的方法,提出了一种制作蓝相Ⅱ态液晶晶格模型的新方法,这种方法可以做出全空间的液晶分子指向矢。利用做出的新模型,采用时域有限差分法(FDTD)进行仿真模拟光学特性,当光源采用圆偏振时,模拟出的结果表明,左旋圆偏振和右旋圆偏振光的透过率有着显著的差别,与蓝相液晶螺旋方向相同的圆偏振光在特定的波长范围会被大量反射。  相似文献   

11.
    
2D Ruddlesden–Popper perovskites are interesting for a variety of applications owing to their tunable optical properties and their excellent ambient stability. As these materials are processable from solution, they hold the promise of procuring flexible and cost‐effective films through large‐scale fabrication techniques. However, such solution‐based deposition techniques often induce large degrees of heterogeneity due to poorly controlled crystallization. The microscopic properties of films of (PEA)2PbI4 cast from precursor solutions of different stoichiometry are therefore investigated. The stoichiometry of the precursor solution is found to have a large impact on the crystallinity, morphology, and optical properties of the resulting thin films. Even for films cast from stoichiometric precursors, differences in photoluminescence intensities occur on a subgranular level. The heterogeneity in these films is found to be thermally activated with an activation energy of 0.4 eV for the emergence of local variations in nonradiative recombination rates. The spatial variation in the distribution of trap states is attributed to local fluctuations in the stoichiometry. In line with this, the surface can successfully be passivated by providing an excess of phenylethylammonium iodide (PEAI) to an as‐cast film, enhancing the photoluminescence by as much as 85% without significantly altering the film's morphology.  相似文献   

12.
    
Copper(I) halides are emerging as attractive alternatives to lead halide perovskites for optical and electronic applications. However, blue-emitting all-inorganic copper(I) halides suffer from poor stability and lack of tunability of their photoluminescence (PL) properties. Here, the preparation of silver(I) halides A2AgX3 (A = Rb, Cs; X = Cl, Br, I) through solid-state synthesis is reported. In contrast to the Cu(I) analogs, A2AgX3 are broad-band emitters sensitive to A and X site substitutions. First-principle calculations show that defect-bound excitons are responsible for the observed main PL peaks in Rb2AgX3 and that self-trapped excitons (STEs) contribute to a minor PL peak in Rb2AgBr3. This is in sharp contrast to Rb2CuX3, in which the PL is dominated by the emission by STEs. Moreover, the replacement of Cu(I) with Ag(I) in A2AgX3 significantly improves photostability and stability in the air under ambient conditions, which enables their consideration for practical applications. Thus, luminescent inks based on A2AgX3 are prepared and successfully used in anti-counterfeiting applications. The excellent light emission properties, significantly improved stability, simple preparation method, and tunable light emission properties demonstrated by A2AgX3 suggest that silver(I) halides may be attractive alternatives to toxic lead halide perovskites and unstable copper(I) halides for optical applications.  相似文献   

13.
    
Rare earth elements are widely employed and investigated as dopants in luminescent materials because of their ability to modulate hosts’ specific physical and chemical properties. However, stable phosphors crystallized with pure rare earth elements are few and hence their potential for wider utilization is largely limited. Herein, two examples of cerium (Ce)-based organic–inorganic hybrid halides, (DFPD)4CeX7 (DFPD+ = 4,4-difluoropiperidinium; X− = Cl− and Br−) and (DFPD)CeCl4·2MeOH are demonstrated. The Cl compositions of both examples are capable of emitting the fascinating ultraviolet (UV) light (350–375 nm), which represents the shortest emission wavelength ever reported in existing metal halide perovskites. Moreover, the resulting crystals are of high quality, which have intrinsic photoluminescence quantum yields of 95%–100%. Besides, in contrast to their all-inorganic counterparts like Ce3CeBr6, the proposed two forms of Ce3+-based halides show abnormal anti-thermal quenching behavior (≈128% of emission intensity at 420 K relative to 80 K), being particularly applicable for practical use in a heated environment. A phosphor-converted light-emitting diode fabricated with (DFPD)4CeCl7 demonstrates stable UV emission (840 min) and has a high external quantum efficiency of 1%. This study opens up the way to a possible design of robust UV-emitting structures based on rare earth hybrid metal halides.  相似文献   

14.
    
Self-healing of defects imposed by external stimuli such as high energy radiation is a possibility to sustain the operational lifetime of electronic devices such as radiation detectors. Cs3Bi2Br3I6 polycrystalline wafers are introduced here as novel X-ray detector material, which not only guarantees a high X-ray stopping power due to its composition with elements with high atomic numbers, but also outperforms other Bi-based semiconductors in respect to detector parameters such as detection limit, transient behavior, or dark current. The polycrystalline wafers represent a size scalable technology suitable for future integration in imager devices for medical applications. Most astonishingly, aging of these wafer-based devices results in an overall improvement of the detector performance—dark currents are reduced, photocurrents are increased, and one of the most problematic properties of X-ray detectors, the base line drift is reduced by orders of magnitude. These aging induced improvements indicate self-healing effects which are shown to result from recrystallization. Optimized synthetic conditions also improve the as prepared X-ray detectors; however, the aged device outperforms all others. Thus, self-healing acts in Cs3Bi2Br3I6 as an optimization tool, which is certainly not restricted to this single compound, it is expected to be beneficial also for many further polycrystalline ionic semiconductors.  相似文献   

15.
    
Metal halide perovskite light-emitting diodes (PeLEDs) are gaining increasing attention as a promising candidate for the new-generation display technology. Although tremendous progress has been witnessed in this field, the device performance of blue PeLEDs still lags far behind that of the green and red counterparts. In this work, an effective interfacial engineering is employed to boost the radiative recombination of blue perovskite film by introducing a multifunctional tetraethyl orthosilicate (TEOS) network on the grain-growth substrate. Benefitting from the strong interaction between the TEOS molecule and perovskite nuclei, the perovskite crystallization dynamics are effectively regulated, contributing to significantly improved emitting film with uniformly distributed halogen and concentrated low-dimensional domain. Additionally, the TEOS network can distinctly passivate the crystal defects at the buried perovskite interface owing to its adequate electron-donating sites. Consequently, the target blue PeLEDs featuring a stable emission peak at 488 nm exhibit a champion external quantum efficiency of 17.3%, which is among the highest values to date. The results demonstrate the critical role of the surface molecular characteristics of the grain-growth substrate in regulating the mixed-halide blue perovskite crystallization.  相似文献   

16.
    
Metal–organic frameworks (MOFs) are highly versatile materials that have been identified as promising candidates for membrane-based gas separation applications due to their uniformly narrow pore windows and virtually unlimited structural and chemical features. Defect engineering of MOFs has opened new opportunities for manipulating MOF structures, providing a simple yet efficient approach for enhancing membrane separation. However, the utilization of this strategy to tailor membrane microstructures and enhance separation performance is still in its infancy. Thus, this summary aims to provide a guideline for tailoring defective MOF-based membranes. Recent developments in defect engineering of MOF-based membranes will be discussed, including the synthesis strategies for defective MOFs, the effects of defects on the gas adsorption properties, gas transport mechanisms, and recently reported defective MOF-based membranes. Furthermore, the emerging challenges and future prospects will be outlined. Overall, defect engineering offers an exciting opportunity to improve the performance of MOF-based gas membranes. However, there is still a long way to go to fully understand the influence of defects on MOF properties and optimize the design of MOF-based membranes for specific gas separation applications. Nonetheless, continued research in this field holds great promise for the development of next-generation membrane-based gas separation technologies.  相似文献   

17.
    
Blue light emitting two dimensional (2D) and quasi‐2D layered halide perovskites (LHPs) are gaining attention in solid‐state lighting applications but their fragile stability in humid condition is one of the most pressing issues for their practical applications. Though water is much greener and cost effective, organic solvents must be used during synthesis as well as the device fabrication process for these LHPs due to their water‐sensitivity/instability and consequently, water‐stable blue‐light emitting 2D and quasi‐2D LHPs have not been documented yet. Here, water‐mediated facile and cost‐effective syntheses, characterizations, and optical properties of 16 organic–inorganic hybrid compounds are reported including 2D (A′)2PbX4 (A′ = butylammonium, X = Cl/Br/I) (8 compounds), 3D perovskites (4), and quasi‐2D (A′)pAx?1BxX3x+1 LHPs (A = methylammonium) (4) in water. Here, both composition and dimension of LHPs are tuned in water, which has never been explored yet. Furthermore, the dual emissive nature is observed in quasi‐2D perovskites, where the intensity of two photoluminescence (PL) peaks are governed by 2D and 3D inorganic layers. The Pb(OH)2‐coated 2D and quasi‐2D perovskites are highly stable in water even after several months. In addition, single particle imaging is performed to correlate structural–optical property of these LHPs.  相似文献   

18.
    
According to the thinner emitting layer and stronger electric field in perovskite light-emitting diodes (PeLEDs) than those in perovskite solar cells, the strong electric-field-driven ion-migration is a key issue for the operational stability of PeLEDs. Here, a methylene-bis-acrylamide cross-linking strategy is proposed to both passivate defects and suppress ion-migration with an emphasis on the suppressing mechanism via in situ investigations. As typical results, in addition to the enhanced external quantum efficiency (EQE, 16.8%), PeLEDs exhibit preferable operational stability with a half lifetime (T50) of 208 h under continuous operation with an initial luminance of 100 cd m−2. Moreover, the EQE of cross-linked LEDs can maintain above 15% during 25 times scanning as the devices are measured every 4 days. To the authors’ knowledge, this is the highest stability published until now for high-efficiency PeLEDs with EQE over 15%. The in situ/ex situ mechanism investigation demonstrates that such cross-linking increases binding energy from 0.54 to 0.92 eV and activation energy from 0.21 to 0.5 eV. Hence, it suppresses ligands breaking away and ion migration, which prevents ions from moving inside and across crystals. The proposed cross-linking passivation strategy thus provides an effective methodology to fabricate stable perovskites-based photoelectric devices.  相似文献   

19.
    
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.  相似文献   

20.
    
The perovskite layer contains a large number of charged defects that seriously impair the efficiency and stability of perovskite solar cells (PSCs), thus it is essential to develop an effective passivation strategy to heal them. Based on theoretical calculations, it is found that enhancing the electrostatic potential of passivators can improve passivation effect and adsorption energy between charged defects and passivators. Herein, an electrostatic potential modulation (EPM) strategy is developed to design passivators for highly efficient and stable PSCs. With the EPM strategy, 1-phenylethylbiguanide (PEBG) and 1-phenylbiguanide (PBG) are designed. It is found that the charge distribution and electrostatic potential of phenyl- and phenylethyl- substituent on the biguanide are significantly enhanced. The N atom directly bonding to the phenyl group shows larger positive charge than that bonding to the phenylethyl group. The modulated electrostatic potential makes PBG bind stronger with the defects on perovskite surface. Based on the effective passivation of EPM, a champion efficiency of 24.67% is realized and the device retain 91.5% of its initial PCE after ≈1300 h. The promising EPM strategy, which provides a principle of passivator design and allows passivation to be controllable, may advance further optimization and application of perovskite solar cells toward commercialization.  相似文献   

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