Perovskite light-emitting diodes based on solution-processed self-organized multiple quantum wells, Nature Photonics, 2016. 10(11) Encouraging performance metrics of light-emitting diodes (LEDs) based on 3Dperovskites, such as low turn-on voltages and external quantum efficiencies (EQEs) of up to 3.5% at high current densities, have been demonstrated 9 . However, the EL quantum efficiency is far behind the limit predicated by ~70% PLQE of the 3D perovskites, mainly due to the existence of current losses caused by incomplete surface coverage of the perovskite films and the fact that the high PLQE can only be obtained at high excitations 8,9 . By using thick (>300 nm) perovskite films, Cho et al.obtained LEDs with over 8% EQE 10 . However, for this device, the turn-on voltage is high and the power efficiency is low, which may result from the thick perovskite layer used. In order to further enhance the performance of 3D perovskite-based LEDs, it is 3 essential to obtain perovskite thin films with both complete surface coverage and high PLQE [8][9][10] . Moreover, device stability, which was proven to be a vital issue in organic-inorganic halide perovskite-based photovoltaics 11 , has not been addressed in perovskite LEDs.The 3D perovskites are actually an extreme case of layered organometal halide perovskites with a general formula of L2(SMX3)n-1MX4, where M, X, L, and S are a divalent metal cation, a halide, and organic cations with long and short chains, respectively ( Fig. 1a) [12][13][14] . Here n is the number of semiconducting MX4 monolayer sheets within the two organic insulating layers (cation L), with n=∞ corresponding to the structure of a 3D perovskite SMX3. With smaller numbers of MX4 layers, quantum confinement effects, such as an increase in bandgap and exciton energy, become important 6,15 . In consequence, the layered perovskites naturally form quantum-well structures. At the opposite extreme, when n=1, the layered perovskites form a monolayer structure of a two-dimensional (2D) perovskite L2MX4. The 2D L2MX4 perovskites generally have good film-formation properties 13 . Nevertheless, the PLQEs of the 2D perovskites are rather low at room temperature, owing to fast exciton quenching rates 6,7 . LEDs based on the 2D perovskites have been attempted, while the devices are either very low in efficiency or only operational at cryogenic temperatures [16][17][18] . Here we demonstrate very efficient (up to 11.7% EQE) and high-brightness EL achievable at room temperature by using solution-processed perovskite multiple quantum wells (MQWs) with an energy cascade, which can combine the advantages of 2D and 3D perovskites. We note, a relevant perovskite LED work 19 which shows a peak EQE of 8.8% has been published online during the revision of this paper.A precursor solution of 1-naphthylmethylamine iodide (NMAI), formamidinium iodide (FAI), and PbI2 with a molar ratio of 2:1:2 dissolved in N,N-dimethylformamide (DMF) was used to deposit perovskite films (see Methods for details), which are abbreviated as NFPI...

Efficiency roll-off is a major issue for most types of light-emitting diodes (LEDs), and its origins remain controversial. Here we present investigations of the efficiency roll-off in perovskite LEDs based on two-dimensional layered perovskites. By simultaneously measuring electroluminescence and photoluminescence on a working device, supported by transient photoluminescence decay measurements, we conclude that the efficiency roll-off in perovskite LEDs is mainly due to luminescence quenching which is likely caused by non-radiative Auger recombination. This detrimental effect can be suppressed by increasing the width of quantum wells, which can be easily realized in the layered perovskites by tuning the ratio of large and small organic cations in the precursor solution. This approach leads to the realization of a perovskite LED with a record external quantum efficiency of 12.7%, and the efficiency remains to be high, at approximately 10%, under a high current density of 500 mA cm −2 .

device stability impedes its commercialization, mainly stemming from the chemical decomposition of regular 3D perovskites in damp environment. [3,4] Encapsulation techniques can slow down the degradation process, but the essential approach to tackle this issue is to find stable perovskite materials capable of achieving long-term stability. [5] In contrast to traditional 3D counterparts, quasi-2D layered perovskites have shown enhanced stability owing to the bulkier and hydrophobic organic molecule in the structure, and have been applied both in photovoltaics and light-emitting diodes. [6][7][8][9] Quasi-2D perovskites take the generic structural formula of L 2 S n−1 M n X 3n+1 , where n is an integer, M is a divalent metal, X is a halide anion, and L and S are organic cations with large and small sizes, respectively. [10] Layered structures are usually formed by inserting the large-sized organic cation spacers into the inorganic sheets of corner-sharing [MX 6 ] octahedra. These quasi-2D compounds can be regarded as natural formed quantum-well (QW) structures, in which the semiconducting inorganic sheets act as the wells and the organic dielectric layers correspond to the Quasi-2D layered organometal halide perovskites have recently emerged as promising candidates for solar cells, because of their intrinsic stability compared to 3D analogs. However, relatively low power conversion efficiency (PCE) limits the application of 2D layered perovskites in photovoltaics, due to large energy band gap, high exciton binding energy, and poor interlayer charge transport. Here, efficient and water-stable quasi-2D perovskite solar cells with a peak PCE of 18.20% by using 3-bromobenzylammonium iodide are demonstrated. The unencapsulated devices sustain over 82% of their initial efficiency after 2400 h under relative humidity of ≈40%, and show almost unchanged photovoltaic parameters after immersion into water for 60 s. The robust performance of perovskite solar cells results from the quasi-2D perovskite films with hydrophobic nature and a high degree of electronic order and high crystallinity, which consists of both ordered large-bandgap perovskites with the vertical growth in the bottom region and oriented smallbandgap components in the top region. Moreover, due to the suppressed nonradiative recombination, the unencapsulated photovoltaic devices can work well as light-emitting diodes (LEDs), exhibiting an external quantum efficiency of 3.85% and a long operational lifetime of ≈96 h at a high current density of 200 mA cm −2 in air.

This paper reports a facile and scalable process to achieve high performance red perovskite light-emitting diodes (LEDs) by introducing inorganic Cs into multiple quantum well (MQW) perovskites. The MQW structure facilitates the formation of cubic CsPbI perovskites at low temperature, enabling the Cs-based QWs to provide pure and stable red electroluminescence. The versatile synthesis of MQW perovskites provides freedom to control the crystallinity and morphology of the emission layer. It is demonstrated that the inclusion of chloride can further improve the crystallization and consequently the optical properties of the Cs-based MQW perovskites, inducing a low turn-on voltage of 2.0 V, a maximum external quantum efficiency of 3.7%, a luminance of ≈440 cd m at 4.0 V. These results suggest that the Cs-based MQW LED is among the best performing red perovskite LEDs. Moreover, the LED device demonstrates a record lifetime of over 5 h under a constant current density of 10 mA cm . This work suggests that the MQW perovskites is a promising platform for achieving high performance visible-range electroluminescence emission through high-throughput processing methods, which is attractive for low-cost lighting and display applications.

3D organometal halide perovskite. [2] Due to the poor film morphology and strong trap-assisted nonradiative recombination, the device performance is modest, with a peak EQE of 0.76%. Many methods, including interfacial engineering, polymer additive, and antisolvent, have been used to improve the quality of perovskite films. [3,[13][14][15] However, due to the serious trap-assisted nonradiative recombination, the photoluminescence quantum efficiencies (PLQEs) of 3D perovskites at low excitations are quite low, limiting the further improvement of device performance.The emerged multiple-quantum-well (MQW) perovskite has the merits of good film morphology and high PLQE, which is promising to achieve high performance LEDs. The MQW perovskite can be defined as quasi-2D layered perovskite, which is composed of different layered perovskites with naturally formed quantum wells (QWs) (Figure 1). [16][17][18] Generally, the layered perovskite has a formula of L 2 (SMX 3 ) n−1 MX 4 , where L is the large organic cation, S is the small monovalent cation, M is the divalent metal cation, X is the halide anion, and n is the number of MX 4 2− sheets. [19][20][21] In layered perovskites, the MX 4 2− sheet acts as potential well and its number, n, determines well width and the bandgap, while the large organic layer acts as potential barrier and its ionic radius determines the barrier width. It was found that quasi-2D layered perovskite thin film can spontaneously form MQW structure by spin-coating process, which is a mixture of layered perovskites with different n numbers and different bandgaps. [16] The energy transfer process from large bandgap QWs to small bandgap QWs is fast and efficient, resulting in carrier localization and accumulation in low energy QWs. [16,18] Consequently, trap-induced nonradiative recombination can be suppressed and high PLQE can be obtained. Based on the MQWs, the EQE of perovskite LEDs first reaches >10% in 2016. [16,22] Recently, through further suppressing nonradiative recombination and enhancing outcoupling by polymer additive, the peak EQE of near-infrared (NIR) perovskite LEDs based on MQWs has reached 20%. [7] Here, we focus on the unique properties of MQW perovskite and address its potential for high performance LEDs. We then discuss how to control the MQW structure and its effect on perovskite LED performance. Why MQW Perovskites are Promising for High Performance LEDsFor perovskite LEDs, the EQE is intrinsically limited by the properties of perovskite film, which also determine the stability Light-emitting diodes (LEDs) based on solution-processed metal halide perovskites have shown great application potential in energy-efficient lighting and displays. Multiple-quantum-well (MQW) perovskites simultaneously possess high photoluminescence quantum efficiency and good film morphology and stability, making it attractive for high-performance perovskite LEDs. Here, merits of MQW perovskites and the progress in MQW perovskite LEDs are reviewed. Challenges and future directions of perovskite LEDs are ...

Solution-processed metal halide perovskites have been recognized as one of the most promising semiconductors, with applications in light-emitting diodes (LEDs), solar cells and lasers. Various additives have been widely used in perovskite precursor solutions, aiming to improve the formed perovskite film quality through passivating defects and controlling the crystallinity. The additive’s role of defect passivation has been intensively investigated, while a deep understanding of how additives influence the crystallization process of perovskites is lacking. Here, we reveal a general additive-assisted crystal formation pathway for FAPbI3 perovskite with vertical orientation, by tracking the chemical interaction in the precursor solution and crystallographic evolution during the film formation process. The resulting understanding motivates us to use a new additive with multi-functional groups, 2-(2-(2-Aminoethoxy)ethoxy)acetic acid, which can facilitate the orientated growth of perovskite and passivate defects, leading to perovskite layer with high crystallinity and low defect density and thereby record-high performance NIR perovskite LEDs (~800 nm emission peak, a peak external quantum efficiency of 22.2% with enhanced stability).

Halide perovskite multiple quantum wells (MQWs) have recently shown great potential in the field of light-emitting diodes. We report a facile solution-based approach to fabricate dimensionality-tunable perovskite MQWs by introducing 1-naphthylmethylammonium (NMA) cations into CsPbI perovskites. Through the dimensional tailoring of (NMA)CsPbI perovskite MQWs, the crystallinity and photoluminescence quantum efficiencies (PLQEs) are significantly improved. We have obtained high-performance red perovskite light-emitting diodes (PeLEDs) with a luminance of 732 cd m and a maximum external quantum efficiency of 7.3%, which are among the best-performing red PeLEDs. Significantly, the maximum luminance of our PeLEDs is obtained at a low applied voltage of 3.4 V, with a turn-on voltage close to the perovskite band gap (V ≈ 1.9 V). These outstanding performance characteristics demonstrate that dimensional tailoring of perovskite MQWs is a feasible and effective strategy to achieve high-performance PeLEDs, which is attractive for full-color display applications of perovskites.

Solution-processed metal-halide perovskites are emerging as one of the most promising materials for displays, lighting and energy generation. Currently, the best-performing perovskite optoelectronic devices are based on lead halides and the lead toxicity severely restricts their practical applications. Moreover, efficient white electroluminescence from broadband-emission metal halides remains a challenge. Here we demonstrate efficient and bright lead-free LEDs based on cesium copper halides enabled by introducing an organic additive (Tween, polyethylene glycol sorbitan monooleate) into the precursor solutions. We find the additive can reduce the trap states, enhancing the photoluminescence quantum efficiency of the metal halide films, and increase the surface potential, facilitating the hole injection and transport in the LEDs. Consequently, we achieve warm-white LEDs reaching an external quantum efficiency of 3.1% and a luminance of 1570 cd m−2 at a low voltage of 5.4 V, showing great promise of lead-free metal halides for solution-processed white LED applications.