Perovskite light-emitting diodes based on spontaneously formed submicrometre-scale structures
TL;DR: The formation of submicrometre-scale structure in perovskite light-emitting diodes can raise their external quantum efficiency beyond 20%, suggesting the possibility of both high efficiency and high brightness.
Abstract: Light-emitting diodes (LEDs), which convert electricity to light, are widely used in modern society—for example, in lighting, flat-panel displays, medical devices and many other situations. Generally, the efficiency of LEDs is limited by nonradiative recombination (whereby charge carriers recombine without releasing photons) and light trapping1–3. In planar LEDs, such as organic LEDs, around 70 to 80 per cent of the light generated from the emitters is trapped in the device4,5, leaving considerable opportunity for improvements in efficiency. Many methods, including the use of diffraction gratings, low-index grids and buckling patterns, have been used to extract the light trapped in LEDs6–9. However, these methods usually involve complicated fabrication processes and can distort the light-output spectrum and directionality6,7. Here we demonstrate efficient and high-brightness electroluminescence from solution-processed perovskites that spontaneously form submicrometre-scale structures, which can efficiently extract light from the device and retain wavelength- and viewing-angle-independent electroluminescence. These perovskites are formed simply by introducing amino-acid additives into the perovskite precursor solutions. Moreover, the additives can effectively passivate perovskite surface defects and reduce nonradiative recombination. Perovskite LEDs with a peak external quantum efficiency of 20.7 per cent (at a current density of 18 milliamperes per square centimetre) and an energy-conversion efficiency of 12 per cent (at a high current density of 100 milliamperes per square centimetre) can be achieved—values that approach those of the best-performing organic LEDs. The formation of submicrometre-scale structure in perovskite light-emitting diodes can raise their external quantum efficiency beyond 20%, suggesting the possibility of both high efficiency and high brightness.
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TL;DR: In this paper, an electron transport layer with an ideal film coverage, thickness and composition was developed by tuning the chemical bath deposition of tin dioxide (SnO2) to improve the performance of metal halide perovskite solar cells.
Abstract: Metal halide perovskite solar cells (PSCs) are an emerging photovoltaic technology with the potential to disrupt the mature silicon solar cell market. Great improvements in device performance over the past few years, thanks to the development of fabrication protocols1-3, chemical compositions4,5 and phase stabilization methods6-10, have made PSCs one of the most efficient and low-cost solution-processable photovoltaic technologies. However, the light-harvesting performance of these devices is still limited by excessive charge carrier recombination. Despite much effort, the performance of the best-performing PSCs is capped by relatively low fill factors and high open-circuit voltage deficits (the radiative open-circuit voltage limit minus the high open-circuit voltage)11. Improvements in charge carrier management, which is closely tied to the fill factor and the open-circuit voltage, thus provide a path towards increasing the device performance of PSCs, and reaching their theoretical efficiency limit12. Here we report a holistic approach to improving the performance of PSCs through enhanced charge carrier management. First, we develop an electron transport layer with an ideal film coverage, thickness and composition by tuning the chemical bath deposition of tin dioxide (SnO2). Second, we decouple the passivation strategy between the bulk and the interface, leading to improved properties, while minimizing the bandgap penalty. In forward bias, our devices exhibit an electroluminescence external quantum efficiency of up to 17.2 per cent and an electroluminescence energy conversion efficiency of up to 21.6 per cent. As solar cells, they achieve a certified power conversion efficiency of 25.2 per cent, corresponding to 80.5 per cent of the thermodynamic limit of its bandgap.
1,557 citations
Center for Advanced Materials1, Linköping University2, Shenzhen University3, Istituto Italiano di Tecnologia4, Nanyang Technological University5, University of Basel6, Swiss Federal Laboratories for Materials Science and Technology7, Nanjing University8, Beihang University9, Northwestern Polytechnical University10
TL;DR: A major efficiency limit for solution-processed perovskite optoelectronic devices, for example light-emitting diodes, is trap-mediated non-radiative losses as mentioned in this paper.
Abstract: A major efficiency limit for solution-processed perovskite optoelectronic devices, for example light-emitting diodes, is trap-mediated non-radiative losses. Defect passivation using organic molecul ...
849 citations
TL;DR: This review summarizes the mechanisms of intrinsic- and extrinsic-environment-induced decomposition of perovskite quantum dots and some possible solutions to improve the stability of PQDs together with suggestions for further improving the performance of pc-LEDs as well as the device lifetime.
Abstract: Beyond the unprecedented success achieved in photovoltaics (PVs), lead halide perovskites (LHPs) have shown great potential in other optoelectronic devices. Among them, nanometer-scale perovskite quantum dots (PQDs) with fascinating optical properties including high brightness, tunable emission wavelength, high color purity, and high defect tolerance have been regarded as promising alternative down-conversion materials in phosphor-converted light-emitting diodes (pc-LEDs) for lighting and next-generation of display technology. Despite the promising applications of perovskite materials in various fields, they have received strong criticism for the lack of stability. The poor stability has also attracted much attention. Within a few years, numerous strategies towards enhancing the stability have been developed. This review summarizes the mechanisms of intrinsic- and extrinsic-environment-induced decomposition of PQDs. Simultaneously, the strategies for improving the stability of PQDs are reviewed in detail, which can be classified into four types: (1) compositional engineering; (2) surface engineering; (3) matrix encapsulation; (4) device encapsulation. Finally, the challenges for applying PQDs in pc-LEDs are highlighted, and some possible solutions to improve the stability of PQDs together with suggestions for further improving the performance of pc-LEDs as well as the device lifetime are provided.
751 citations
TL;DR: In this paper, the predominant pathways that contribute to non-radiative recombination losses in perovskite solar cells, and evaluate their impact on device performance are analyzed, and some notable advances in mitigating these losses are highlighted.
Abstract: Photovoltaic solar cells based on metal halide perovskites have gained considerable attention over the past decade because of their potentially low production cost, earth-abundant raw materials, ease of fabrication and ever-increasing power conversion efficiencies of up to 25.2%. This type of solar cells offers the promise of generating electricity at a more competitive unit price than traditional fossil fuels by 2035. Nevertheless, the best research cell efficiencies are still below the theoretical limit defined by the Shockley-Queissier theory owing to the presence of non-radiative recombination losses. In this Review, we analyse the predominant pathways that contribute to non-radiative recombination losses in perovskite solar cells, and evaluate their impact on device performance. We then discuss how non-radiative recombination losses can be estimated through reliable characterization techniques, and highlight some notable advances in mitigating these losses, which hint at pathways towards defect-free perovskite solar cells. Finally, we outline directions for future work that will push the efficiency of perovskite solar cells towards the radiative limit.
644 citations
TL;DR: The development of perovskite emitters, their use in light-emitting devices, and the challenges in enhancing the efficiency and stability, as well as reducing the potential toxicity of this technology are discussed in this Review.
Abstract: Metal halide perovskites have shown promising optoelectronic properties suitable for light-emitting applications. The development of perovskite light-emitting diodes (PeLEDs) has progressed rapidly over the past several years, reaching high external quantum efficiencies of over 20%. In this Review, we focus on the key requirements for high-performance PeLEDs, highlight recent advances on materials and devices, and emphasize the importance of reliable characterization of PeLEDs. We discuss possible approaches to improve the performance of blue and red PeLEDs, increase the long-term operational stability and reduce toxicity hazards. We also provide an overview of the application space made possible by recent developments in high-efficiency PeLEDs. The development of perovskite emitters, their use in light-emitting devices, and the challenges in enhancing the efficiency and stability, as well as reducing the potential toxicity of this technology are discussed in this Review.
602 citations
References
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TL;DR: It is shown, using photoluminescence studies, that radiative bimolecular recombination is dominant at higher excitation densities, Hence, the quantum efficiencies of the perovskite light-emitting diodes increase at higher current densities.
Abstract: Solid-state light-emitting devices based on direct-bandgap semiconductors have, over the past two decades, been utilized as energy-efficient sources of lighting. However, fabrication of these devices typically relies on expensive high-temperature and high-vacuum processes, rendering them uneconomical for use in large-area displays. Here, we report high-brightness light-emitting diodes based on solution-processed organometal halide perovskites. We demonstrate electroluminescence in the near-infrared, green and red by tuning the halide compositions in the perovskite. In our infrared device, a thin 15 nm layer of CH3NH3PbI(3-x)Cl(x) perovskite emitter is sandwiched between larger-bandgap titanium dioxide (TiO2) and poly(9,9'-dioctylfluorene) (F8) layers, effectively confining electrons and holes in the perovskite layer for radiative recombination. We report an infrared radiance of 13.2 W sr(-1) m(-2) at a current density of 363 mA cm(-2), with highest external and internal quantum efficiencies of 0.76% and 3.4%, respectively. In our green light-emitting device with an ITO/PEDOT:PSS/CH3NH3PbBr3/F8/Ca/Ag structure, we achieved a luminance of 364 cd m(-2) at a current density of 123 mA cm(-2), giving external and internal quantum efficiencies of 0.1% and 0.4%, respectively. We show, using photoluminescence studies, that radiative bimolecular recombination is dominant at higher excitation densities. Hence, the quantum efficiencies of the perovskite light-emitting diodes increase at higher current densities. This demonstration of effective perovskite electroluminescence offers scope for developing this unique class of materials into efficient and colour-tunable light emitters for low-cost display, lighting and optical communication applications.
3,466 citations
TL;DR: A perovskite solar cell that uses a double layer of mesoporous TiO2 and ZrO2 as a scaffold infiltrated with perovSkite and does not require a hole-conducting layer is fabricated and achieves a certified power conversion efficiency of 12.8%.
Abstract: We fabricated a perovskite solar cell that uses a double layer of mesoporous TiO2 and ZrO2 as a scaffold infiltrated with perovskite and does not require a hole-conducting layer. The perovskite was produced by drop-casting a solution of PbI2, methylammonium (MA) iodide, and 5-ammoniumvaleric acid (5-AVA) iodide through a porous carbon film. The 5-AVA templating created mixed-cation perovskite (5-AVA)x(MA)1- xPbI3 crystals with lower defect concentration and better pore filling as well as more complete contact with the TiO2 scaffold, resulting in a longer exciton lifetime and a higher quantum yield for photoinduced charge separation as compared to MAPbI3. The cell achieved a certified power conversion efficiency of 12.8% and was stable for >1000 hours in ambient air under full sunlight.
2,639 citations
TL;DR: This optoelectronic performance is achieved by inserting an insulating layer between the quantum dot layer and the oxide electron-transport layer to optimize charge balance in the device and preserve the superior emissive properties of the quantum dots.
Abstract: Solution-processed optoelectronic and electronic devices are attractive owing to the potential for low-cost fabrication of large-area devices and the compatibility with lightweight, flexible plastic substrates. Solution-processed light-emitting diodes (LEDs) using conjugated polymers or quantum dots as emitters have attracted great interest over the past two decades. However, the overall performance of solution-processed LEDs--including their efficiency, efficiency roll-off at high current densities, turn-on voltage and lifetime under operational conditions-remains inferior to that of the best vacuum-deposited organic LEDs. Here we report a solution-processed, multilayer quantum-dot-based LED with excellent performance and reproducibility. It exhibits colour-saturated deep-red emission, sub-bandgap turn-on at 1.7 volts, high external quantum efficiencies of up to 20.5 per cent, low efficiency roll-off (up to 15.1 per cent of the external quantum efficiency at 100 mA cm(-2)), and a long operational lifetime of more than 100,000 hours at 100 cd m(-2), making this device the best-performing solution-processed red LED so far, comparable to state-of-the-art vacuum-deposited organic LEDs. This optoelectronic performance is achieved by inserting an insulating layer between the quantum dot layer and the oxide electron-transport layer to optimize charge balance in the device and preserve the superior emissive properties of the quantum dots. We anticipate that our results will be a starting point for further research, leading to high-performance, all-solution-processed quantum-dot-based LEDs ideal for next-generation display and solid-state lighting technologies.
1,958 citations
TL;DR: It is shown that surface modifiers based on polymers containing simple aliphatic amine groups substantially reduce the work function of conductors including metals, transparent conductive metal oxides, conducting polymers, and graphene.
Abstract: Organic and printed electronics technologies require conductors with a work function that is sufficiently low to facilitate the transport of electrons in and out of various optoelectronic devices. We show that surface modifiers based on polymers containing simple aliphatic amine groups substantially reduce the work function of conductors including metals, transparent conductive metal oxides, conducting polymers, and graphene. The reduction arises from physisorption of the neutral polymer, which turns the modified conductors into efficient electron-selective electrodes in organic optoelectronic devices. These polymer surface modifiers are processed in air from solution, providing an appealing alternative to chemically reactive low–work function metals. Their use can pave the way to simplified manufacturing of low-cost and large-area organic electronic technologies.
1,870 citations
1,856 citations