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1.
With respect to three‐dimensional (3D) perovskites, quasi‐two‐dimensional (quasi‐2D) perovskites have unique advantages in light‐emitting devices (LEDs), such as strong exciton binding energy and good phase stability. Interlayer ligand engineering is a key issue to endow them with these properties. Rational design principles for interlayer materials and their processing techniques remain open to investigation. A co‐interlayer engineering strategy is developed to give efficient quasi‐2D perovskites by employing phenylbutylammonium bromide (PBABr) and propylammonium bromide (PABr) as the ligand materials. Preparation of these co‐interlayer quasi‐2D perovskite films is simple and highly controllable without using antisolvent treatment. Crystallization and morphology are readily manipulated by tuning the ratio of co‐interlayer components. Various optical techniques, including steady and ultrafast transient absorption and photoluminescence spectroscopies, are used to investigate their excitonic properties. Photoluminescence quantum yield (PLQY) of the perovskite film is dramatically improved to 89% due to the combined optimization of exciton binding energy and suppression of trap state formation. Accordingly, a high current efficiency of 66.1 cd A?1 and an external quantum efficiency of 15.1% are achieved for green co‐interlayer quasi‐2D perovskite LEDs without using any light out‐coupling techniques, indicating that co‐interlayer engineering is a simple and effective approach to develop high‐performance perovskite electroluminescence devices.  相似文献   

2.
Quasi‐2D (Q2D) lead halide perovskites have emerged as promising materials for light‐emitting diodes (LEDs) due to their tunable emission, slowed‐down carrier diffusion, and improved stability. However, they are primarily fabricated through solution methods, which hinders its large‐scale manufacture and practical applications. Physical‐vapor‐deposition (PVD) methods have well demonstrated the capability for reproducible, scalable, and layer‐by‐layer fabrication of high quality organic/inorganic thin films. Herein, for the first time, the full‐evaporation fabrication of organic–inorganic hybrid ((BA)2Csn?1PbnBr3n+1) Q2D–3D PeLEDs is demonstrated. The morphology and crystal phase of the perovskite are controlled from 3D to 2D by modulating material composition, annealing temperature, and film thicknesses. The confinement of carriers in 3D layers and the energy funnel effect are discovered and discussed. Importantly, a record high external quantum efficiency (EQE) of 5.3% based on evaporation method is achieved. Moreover, a centimeter‐scale PeLED (1.5 cm × 2 cm) is obtained. Furthermore, the T50 lifetime of the device with an initial brightness of 100 cd m?2 is found to be 90 min with a thin layer PMMA passivation, which is among the longest for all PVD processed PeLEDs. Overall, this work casts a solid stepping stone towards the fabrication of high‐performance PeLEDs on a large‐scale.  相似文献   

3.
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.  相似文献   

4.
2D perovskite is an organic–inorganic hybrid material with good photoelectric properties, generally prepared by using organic groups as isolation molecules. In this study, using manganese chloride and potassium halide as raw materials, all-inorganic 2D lead-free perovskites are prepared by the Bridgeman melting and cooling method. Different from the 2D perovskites synthesized by organic spacer molecules, the prepared all-inorganic 2D perovskites have smaller layer spacings and good crystallization performance due to the use of potassium halide as spacer molecules. They are direct bandgap semiconductors and their energy bandgaps are tuned by the different types of potassium halides. High degree orientation crystal thin films with (001) lattice plane parallel to silicon wafer substrate are prepared by double-source evaporation. The physical morphology of the films is characterized by grazing angle X-ray diffraction, transmission electron microscopy, and electron diffraction. The field effect transistors prepared from these 2D films show excellent electronic characteristics. The mobility of the optimized device is ≈24 cm2 v−1 s−1 and the on/off ratio reaches 105. This study reveals the potential of lead-free manganese 2D perovskite as a high-performance perovskite field effect transistor.  相似文献   

5.
Organic–inorganic hybrid perovskites (OHPs) are promising emitters for light‐emitting diodes (LEDs) due to the high color purity, low cost, and simple synthesis. However, the electroluminescent efficiency of polycrystalline OHP LEDs (PeLEDs) is often limited by poor surface morphology, small exciton binding energy, and long exciton diffusion length of large‐grain OHP films caused by uncontrolled crystallization. Here, crystallization of methylammonium lead bromide (MAPbBr3) is finely controlled by using a polar solvent‐soluble self‐doped conducting polymer, poly(styrenesulfonate)‐grafted polyaniline (PSS‐g‐PANI), as a hole injection layer (HIL) to induce granular structure, which makes charge carriers spatially confined more effectively than columnar structure induced by the conventional poly(3,4‐ethylenedioythiphene):polystyrenesulfonate (PEDOT:PSS). Moreover, lower acidity of PSS‐g‐PANI than PEDOT:PSS reduces indium tin oxide (ITO) etching, which releases metallic In species that cause exciton quenching. Finally, doubled device efficiency of 14.3 cd A‐1 is achieved for PSS‐g‐PANI‐based polycrystalline MAPbBr3 PeLEDs compared to that for PEDOT:PSS‐based PeLEDs (7.07 cd A‐1). Furthermore, PSS‐g‐PANI demonstrates high efficiency of 37.6 cd A‐1 in formamidinium lead bromide nanoparticle LEDs. The results provide an avenue to both control the crystallization kinetics and reduce the migration of In released from ITO by forming OIP films favorable for more radiative luminescence using the polar solvent‐soluble and low‐acidity polymeric HIL.  相似文献   

6.
Solution‐processed and low‐temperature Sn‐rich perovskites show their low bandgap of about 1.2 eV, enabling potential applications in next‐generation cost‐effective ultraviolet (UV)–visible (vis)–near infrared (NIR) photodetection. Particularly, the crystallization (crystallinity and orientation) and film (smooth and dense film) properties of Sn‐rich perovskites are critical for efficient photodetectors, but are limitedly studied. Here, controllable crystallization for growing high‐quality films with the improvements of increased crystallinity and strengthened preferred orientation through a introducing rubidium cation into the methylammonium Sn‐Pb perovskite system (65% Sn) is achieved. Fundamentally, the theoretical results show that rubidium incorporation causes lower surface energy of (110) plane, facilitating growth in the dominating plane and suppressing growth of other competing planes. Consequently, the methylammonium‐rubidium Sn‐Pb perovskite photodetectors simultaneously achieve larger photocurrent and lower noise current. Finally, highly efficient UV–vis–NIR (300–1100 nm) photodetectors with record‐high linear dynamic range of 110 and 3 dB cut‐off frequency reaching 1 MHz are demonstrated. This work contributes to enriching the cation selection in Sn‐Pb perovskite systems and offering a promising candidate for low‐cost UV–vis–NIR photodetection.  相似文献   

7.
Organometal halide perovskites quantum dots (OHP‐QDs) with bright, color‐tunable, and narrow‐band photoluminescence have significant advantages in display, lighting, and laser applications. Due to sparse concentrations and difficulties in the enrichment of OHP‐QDs, production of large‐area uniform films of OHP‐QDs is a challenging task, which largely impedes their use in electroluminescence devices. Here, a simple dip‐coating method has been reported to effectively fabricate large‐area uniform films of OHP‐QDs. Using this technique, multicolor OHP‐QDs light‐emitting diodes (OQ‐LEDs) emitting in blue, blue‐green, green, orange, and red color have been successfully produced by simply tuning the halide composition or size of QDs. The blue, green, and red OQ‐LEDs exhibited, respectively, a maximum luminance of 2673, 2398, and 986 cd m?2 at a current efficiency of 4.01, 3.72, and 1.52 cd A?1, and an external quantum efficiency of 1.38%, 1.06%, and 0.53%, which are much better than most LEDs based on OHP films. The packaged OQ‐LEDs show long‐term stability in air (humidity ≈50%) for at least 7 d. The results demonstrate the great potential of the dip‐coating method to fabricate large‐area uniform films for various QDs. The high‐efficiency OQ‐LEDs also demonstrate the promising potential of OHP‐QDs for low‐cost display, lighting, and optical communication applications.  相似文献   

8.
Quasi‐2D metal halide perovskite films are promising for efficient light‐emitting diodes (LEDs), because of their efficient radiative recombination and suppressed trap‐assisted quenching compared with pure 3D perovskites. However, because of the multidomain polycrystalline nature of solution‐processed quasi‐2D perovskite films, the composition engineering always impacts the emitting properties with complicated mechanisms. Here, defect passivation and domain distribution of quasi‐2D perovskite films prepared with various precursor compositions are systematically studied. As a result, in perovskite films prepared from stoichiometric quasi‐2D precursor compositions, large organic ammonium cations function well as passivators. In comparison, precursor compositions of simply adding large organic halide salt into a 3D perovskite precursor ensure not only the defect passivation but also the effective formation of quasi‐2D perovskite domains, avoiding unfavorable appearance of low‐order domains. Quasi‐2D perovskite films fabricated with a well‐designed precursor composition achieve a high photoluminescence quantum yield of 95.3% and an external quantum efficiency of 14.7% in LEDs.  相似文献   

9.
Lead‐free halide double perovskites with diverse electronic structures and optical responses, as well as superior material stability show great promise for a range of optoelectronic applications. However, their large bandgaps limit their applications in the visible light range such as solar cells. In this work, an efficient temperature‐derived bandgap modulation, that is, an exotic fully reversible thermochromism in both single crystals and thin films of Cs2AgBiBr6 double perovskites is demonstrated. Along with the thermochromism, temperature‐dependent changes in the bond lengths of Ag? Br (RAg? Br) and Bi? Br (RBi? Br) are observed. The first‐principle molecular dynamics simulations reveal substantial anharmonic fluctuations of the RAg? Br and RBi? Br at high temperatures. The synergy of anharmonic fluctuations and associated electron–phonon coupling, and the peculiar spin–orbit coupling effect, is responsible for the thermochromism. In addition, the intrinsic bandgap of Cs2AgBiBr6 shows negligible changes after repeated heating/cooling cycles under ambient conditions, indicating excellent thermal and environmental stability. This work demonstrates a stable thermochromic lead‐free double perovskite that has great potential in the applications of smart windows and temperature sensors. Moreover, the findings on the structure modulation‐induced bandgap narrowing of Cs2AgBiBr6 provide new insights for the further development of optoelectronic devices based on the lead‐free halide double perovskites.  相似文献   

10.
Moisture‐delicate and water‐unstable organic–inorganic halide perovskites (OI‐HPs) create huge challenges for the synthesis of highly efficient water‐stable light‐emitting materials for optoelectronic devices. Herein, a simple acid solution–assisted method to synthesize quantum confined 2D lead perovskites through Mn doping is reported. The efficient energy transfer between host and dopant ions in orange light‐emitting Mn2+‐doped OI‐HPs leads to the most efficient integrated luminescence with a photoluminescence quantum yield over 45%. The Mn2+ substitution of Pb2+ and passivation with low dielectric constant molecules such as phenethylamine, benzylamine, and butylamine enhance water resistivity, leading to water stability. The dual emission process of this water‐stable 2D Mn‐doped perovskite will help in developing highly efficient 2D water‐stable perovskites for practical applications.  相似文献   

11.
Heterogeneous organic-inorganic halide perovskites possess inherent non-uniformities in bandgap that are sometimes engineered and exploited on purpose, like in quasi-2D perovskites. In these systems, charge carrier and excitation energy migration to lower-bandgap sites are key processes governing luminescence. The question, which of them dominates in particular materials and under specific experimental conditions, still remains unanswered, especially when charge carriers comprise excitons. In this study transient absorption (TA) and transient photoluminescence (PL) techniques are combined to address the excited state dynamics in quasi-2D and other heterogeneous perovskite structures in broad temperature range, from room temperature down to 15 K. The data provide clear evidence that charge carrier transfer rather than energy migration dominates in heterogeneous quasi-2D perovskite films.  相似文献   

12.
Here, a detailed characterization of the optical gain properties of sky‐blue‐light‐emitting pyrene‐cored 9,9‐dialkylfluorene starbursts is reported; it is shown that these materials possess encouragingly low laser thresholds and relatively high thermal and environmental stability. The materials exhibit high solid‐state photoluminescence (PL) quantum efficiencies (>90%) and near‐single‐exponential PL decay transients with excited state lifetimes of ~1.4 ns. The thin‐film slab waveguide amplified spontaneous emission (ASE)‐measured net gain reaches 75–78 cm?1. The ASE threshold energy is found to remain unaffected by heating at temperatures up to 130 °C, 40 to 50 °C above Tg. The ASE remained observable for annealing temperatures up to 170 or 200 °C. 1D distributed feedback lasers with 75% fill factor and 320 nm period show optical pumping thresholds down to 38–65 Wcm?2, laser slope efficiencies up to 3.9%, and wavelength tuning ranges of ~40 nm around 471–512 nm. In addition, these lasers have relatively long operational lifetimes, with N1/2 ≥ 1.1 × 105 pulses for unencapsulated devices operated at ten times threshold in air.  相似文献   

13.
A family of trigonal starburst conjugated molecules (TrFPy, TrFPy, and TrF2Py) composed of a truxene core and pyrene cappers with various bridge lengths is synthesized and characterized. The incorporation of pyrene cappers successfully depress the crystallization tendency, resulting in enhanced glassy temperature and improved morphological stability of the thin films. The high photoluminescence yield in neat films and excellent thermal stability render these pyrene‐capped starbursts promising lasing optical gain media. Low amplified spontaneous emission (ASE) thresholds (EthASE) of 180 nJ pulse‐1 and 101 nJ pulse–1 were recorded for TrFPy and TrF2Py, respectively. One dimensional distributed feedback (1D DFB) lasers demonstrated lasing threshold of 9.3 kW/cm2 and 7.3 kW/cm2 for TrFPy (at 457 nm) and TrF2Py lasers (at 451 nm), respectively. The ASE performance of TrFPy and TrF2Py in an ambient condition was recorded with various annealing temperature (from 80 to 250 °C, 10 min). Surprisingly, TrFPy exhibited excellent ASE stability in an ambient condition, which is still detectable even after annealing at 250 °C for 10 min. The results suggest the pyrene‐capped molecular design strategy is positive on improving the optical gain stability and meanwhile maintaining excellent lasing properties.  相似文献   

14.
By doping 2,7‐bis[4‐(N‐carbazole)phenylvinyl]‐9,9′‐spirobifluorene (spiro‐SBCz) into a wide energy gap 4,4′‐bis(9‐carbazole)‐2,2′‐biphenyl (CBP) host, we demonstrate an extremely low ASE threshold of Eth = (0.11 ± 0.05) μJ cm–2 (220 W cm–2) which is the lowest ASE threshold ever reported. In addition, we confirmed that the spiro‐SBCz thin film functions as an active light emitting layer in organic light‐emitting diode (OLED) and a field‐effect transistor (FET). In particular, we succeeded to obtain linear electroluminescence in the FET structure which will be useful for future organic laser diodes.  相似文献   

15.
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.  相似文献   

16.
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.  相似文献   

17.
The two‐step conversion process consisting of metal halide deposition followed by conversion to hybrid perovskite has been successfully applied toward producing high‐quality solar cells of the archetypal MAPbI3 hybrid perovskite, but the conversion of other halide perovskites, such as the lower bandgap FAPbI3, is more challenging and tends to be hampered by the formation of hexagonal nonperovskite polymorph of FAPbI3, requiring Cs addition and/or extensive thermal annealing. Here, an efficient room‐temperature conversion route of PbI2 into the α‐FAPbI3 perovskite phase without the use of cesium is demonstrated. Using in situ grazing incidence wide‐angle X‐ray scattering (GIWAXS) and quartz crystal microbalance with dissipation (QCM‐D), the conversion behaviors of the PbI2 precursor from its different states are compared. α‐FAPbI3 forms spontaneously and efficiently at room temperature from P2 (ordered solvated polymorphs with DMF) without hexagonal phase formation and leads to complete conversion after thermal annealing. The average power conversion efficiency (PCE) of the fabricated solar cells is greatly improved from 16.0(±0.32)% (conversion from annealed PbI2) to 17.23(±0.28)% (from solvated PbI2) with a champion device PCE > 18% due to reduction of carrier recombination rate. This work provides new design rules toward the room‐temperature phase transformation and processing of hybrid perovskite films based on FA+ cation without the need for Cs+ or mixed halide formulation.  相似文献   

18.
The recent development of quasi‐2D perovskite solar cells have drawn significant attention due to the improved stability of these materials and devices against moisture compared to their 3D counterparts. However, the optoelectronic properties of 2D perovskites need to be optimized in order to achieve high efficiency. In this work, the effect of spacer cations, i.e., phenethylammonium (PEA), 4‐fluorophenethylammonium (F‐PEA), and 4‐methoxyphenethylammonium (MeO‐PEA) on the optoelectronic properties and device performance of quasi‐2D perovskites is systematically studied. It is observed that both larger and more hydrophobic cations can improve perovskite stability against moisture, while larger size can adversely influence the device performance. Interestingly, with F‐PEA or MeO‐PEA, distribution of n value can be shifted toward high 3D content in quasi‐2D perovskite layers, which enables lower bandgaps and possibly lower exciton binding energy. Due to the best charge transport and lowest bandgap, the F‐PEAI‐based quasi‐2D perovskite (n = 5) solar cell shows a highest power conversion efficiency (PCE) of 14.5% with excellent stability in air with a humidity of 40–50%, keeping 90% of the original PCE after 40 d. It is believed that the approach may open a way for the design of new organic spacer cations for stable low‐dimensional hybrid perovskites with high performance.  相似文献   

19.
Efficient organic–inorganic metal halide perovskite absorbers have gained tremendous research interest in the past decade due to their super optoelectronic properties and defect tolerance. Lead (Pb) halide perovskites enable highly efficient perovskite solar cells (PSCs) with a record power conversion efficiency (PCE) of over 23%. However, the energy bandgaps of Pb halide perovskites are larger than the optimal bandgap for single junction solar cells, governed by the Shockley–Queisser (SQ) radiative limit. Mixed tin (Sn)‐Pb halide perovskites have drawn significant attention, since their bandgap can be tuned to below 1.2 eV, which opens a door for fabricating all‐perovskite tandem solar cells that can break the SQ radiative limit. This review summarizes the development of low‐bandgap mixed Sn‐Pb PSCs and their applications in all‐perovskite tandem solar cells. Its aim is to facilitate the development of new approaches to achieve high efficiency low‐bandgap single‐junction mixed Sn‐Pb PSCs and all‐perovskite tandem solar cells.  相似文献   

20.
Organolead halide perovskites (OHPs) have shown unprecedented potentials in optoelectronics. However, the inherent large bandgap has restrained its working wavelength within 280–800 nm, while light at other regions, e.g., near‐infrared (NIR), may cause drastic thermal heating effect that goes against the duration of OHP devices, if not properly exploited. Herein, a solution processable and large‐scale synthesis of multifunctional OHP composites containing lanthanide‐doped upconversion nanoparticles (UCNPs) is reported. Upon NIR illumination, the upconverted photons from UCNPs at 520–550 nm can be efficiently absorbed by closely surrounded OHP nanowires (NWs) and photocurrent is subsequently generated. The narrow full width at half maximum of the absorption of rare earth ions (Yb3+ and Er3+) has ensured high‐selective NIR response. Lifetime characterizations have suggested that Förster resonance energy transfer with an efficiency of 28.5% should be responsible for the direct energy transfer from UCNPs to OHP NWs. The fabricated proof‐of‐concept device has showcased perfect response to NIR light at 980 and 1532 nm, which has paved new avenues for applications of such composites in remote control, distance measurement, and stealth materials.  相似文献   

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