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...
Organic-inorganic hybrid perovskite materials have been receiving considerable attention due to their promising applications in many optoelectronic fields. However, some of the fundamental properties of perovskite materials are still disputed, because most of them are derived from a thin-film state. To comprehend the intrinsic characteristics in a single crystal, herein we report, for the first time, the bulk crystal growth of CH 3 NH 3 PbI 3 . Single crystals of tetragonal CH 3 NH 3 PbI 3 with dimensions of 10 mm × 10 mm × 8 mm were grown by a temperature-lowering method in HI solution. Studies in to the refinement and orientations of the CH 3 NH 3 PbI 3 single crystal structure were conducted based on a high quality crystal.The absorption edge of a CH 3 NH 3 PbI 3 single crystal was located at about 836 nm, indicating that the band gap of CH 3 NH 3 PbI 3 is approximately 1.48 eV, which is close to the theoretical results and smaller than those derived from polycrystalline and thin-films. CH 3 NH 3 PbI 3 crystal exhibits a relatively wide absorption (from 250 nm to 800 nm) and a relatively good thermal stability. CrystEngCommThis journal is † Electronic supplementary information (ESI) available. CCDC 1029776; the images of white MAI, white with yellow MAI and residue light yellow PbI 2 ; powder X-ray diffraction patterns for MAI; 1 H-NMR and 13 C-NMR spectra of MAI; selected bond lengthIJÅ) and bond anglesIJdeg) for β-MAPbI 3 , isotropic and anisotropic displacement parameters of MAPbI 3 . See
We report a facile solution-based approach to the in situ growth of perovskite films consisting of monolayers of CsPbBr nanoplates passivated by bulky phenylbutylammonium (PBA) cations, that is, two-dimensional layered PBA(CsPbBr)PbBr perovskites. Optimizing film formation processes leads to layered perovskites with controlled n values in the range of 12-16. The layered perovskite emitters show quantum-confined band gap energies with a narrow distribution, suggesting the formation of thickness-controlled quantum-well (TCQW) structures. The TCQW CsPbBr films exhibit smooth surface features, narrow emission line widths, low trap densities, and high room-temperature photoluminance quantum yields, resulting in high-color-purity green light-emitting diodes (LEDs) with remarkably high external quantum efficiencies (EQEs) of up to 10.4%. The solution-based approach is extended to the preparation of TCQW CsPbI films for high-color-purity red perovskite LEDs with high EQEs of up to 7.3%.
Inorganic−organic hybrid perovskites have drawn considerable attention in photovoltaics and light-emitting diodes (LEDs) due to their exceptional optoelectronic properties. Perovskite multiple quantum wells (MQWs), which employ large organic ammonium cations to form layered structures, have been developed for high-efficiency perovksite LEDs (PeLEDs). However, little is known about the impacts of large organic ammonium cations on the properties of MQW films. In this work, we report MQW perovskites of phenylbutylammonium-cesium lead iodides, which exhibit a photoluminescence peak at 664 nm with a quantum efficiency of 58%. These perovskite MQW films enable red LEDs with high external quantum efficiencies (EQEs) of up to 13.3%. Furthermore, we deposit MQW perovskites of butylammonium-cesium lead iodides. The comparisons of the two perovskite MQW films demonstrate that the choices of large organic ammonium cations significantly influence the properties of the perovskite MQW films, that is, distributions of the quantum-well thicknesses, energy transfer processes, and recombination channels of the emissive centers. Our study shall shed light on the rational design of highperformance perovskite MQW films toward their potential application as red light sources.
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