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1.
Sci Adv ; 10(18): eadn5683, 2024 May 03.
Artículo en Inglés | MEDLINE | ID: mdl-38701203

RESUMEN

Perovskite light-emitting diodes (PeLEDs) have attracted great attention in recent years; however, the halogen vacancy defects in perovskite notably hamper the development of high-efficiency devices. Previously, large-sized passivation agents have been usually used, while the effect of defect passivation is limited due to the weak bonding or the large space steric hindrance. Here, we predict that the ultrasmall-sized formate (Fa) and acetate (Ac) have more efficient passivation ability because of the stronger binding with the perovskite, as demonstrated by density functional theory calculation. We introduce ultrasmall-sized cesium salts (CsFa/CsAc) into buried interface, which can also diffuse into the bulk, resulting in both buried interface and bulk passivation. In addition, the improved perovskite growth has been found due to the enhanced hydrophily after introducing CsFa/CsAc as additive. According to these advantages, a pure-red PeLED with 24.2% efficiency at 639 nm has been achieved.

2.
Nano Lett ; 22(20): 8266-8273, 2022 Oct 26.
Artículo en Inglés | MEDLINE | ID: mdl-36251485

RESUMEN

It is still challenging to achieve high-efficiency pure-red (620-650 nm wavelength) perovskite light-emitting diodes (PeLEDs). Herein, we report pure-red PeLEDs with Commission Internationale de l'Eclairage coordinates (0.703, 0.297) meeting the Rec. 2020, an external quantum efficiency of 20.8%, and a luminance of 3775 cd/m2. This design is based on the strong quantum confinement CsPbI3 quantum dots (QDs) capped by composite ligands of 3-phenyl-1-propylamine and tetrabutylammonium iodide. This strategy stabilized the structure of the strong-confined QDs and reduced the influence of the electric field-induced Stark effect on the PeLEDs. Furthermore, the exciton binding energy of the QDs was decreased by the composited ligands to suppress Auger recombination within the devices. Additionally, the valence-band maximum of the QDs was lifted to match the hole-transport layer, thus balancing charge injection in the PeLEDs. Our device also demonstrated a stable electroluminescence spectrum and a lifetime of 5.6 times longer than the control device.

3.
Adv Mater ; 34(36): e2204460, 2022 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-35855612

RESUMEN

Perovskite light-emitting diodes (PeLEDs) have received great attention in recent years due to their narrow emission bandwidth and tunable emission spectrum. Efficient red emission is one of most important parts for lighting and displays. Quasi-2D perovskites can deliver high emission efficiency due to the strong carrier confinement, while the external quantum efficiencies (EQE) of red quasi-2D PeLEDs are inefficient at present, which is due to the complex distribution of different n-value phases in quasi-2D perovskite films. In this work, the phase distribution of the quasi-2D perovskite is finely controlled by mixing two different large organic cations, which effectively reduces the amount of smaller n-index phases, meanwhile the passivation of lead and halide defects in perovskite films is realized. Accordingly, the PeLEDs show 25.8% EQE and 1300 cd m-2 maximum brightness at 680 nm, which exhibits the highest performance for red PeLEDs up to now.

4.
Small Methods ; 5(8): e2100517, 2021 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-34927872

RESUMEN

Photodetectors with broadband response spectrum have attracted great interest in many application areas such as imaging, gas sensing, and night vision. Here, a high performance broadband photodetector is demonstrated with inorganic perovskite CsPbBr3 /GeSn heterojunction, detection range can be covered from 450 to 2200 nm. The responsivity of heterojunction device can achieve as high as 129 mA W-1 under illuminated light of 532 nm, which is 4.92 times larger than that of a GeSn based device. As the CsPbBr3 can also act as anti-reflective coating for infrared wavelength, the infrared band responsivity at wavelength of 2200 nm can also be raised by 1.42 times. In addition, the device with all inorganic components is showed good stability, while keeping in the dry environment, the device can sustain its 90% original after 550 h storage. These results show the inorganic perovskite/GeSn heterojunction device is of great potential in broadband photodetection with high responsivity.

5.
Adv Mater ; 33(18): e2007169, 2021 May.
Artículo en Inglés | MEDLINE | ID: mdl-33797133

RESUMEN

Perovskite light-emitting diodes (PeLEDs) are considered as particularly attractive candidates for high-quality lighting and displays, due to possessing the features of wide gamut and real color expression. However, most PeLEDs are made from polycrystalline perovskite films that contain a high concentration of defects, including point and extended imperfections. Reducing and mitigating non-radiative recombination defects in perovskite materials are still crucial prerequisites for achieving high performance in light-emitting applications. Here, ethoxylated trimethylolpropane triacrylate (ETPTA) is introduced as a functional additive dissolved in antisolvent to passivate surface and bulk defects during the spinning process. The ETPTA can effectively decrease the charge trapping states by passivation and/or suppression of defects. Eventually, the perovskite films that are sufficiently passivated by ETPTA make the devices achieve a maximum external quantum efficiency (EQE) of 22.49%. To our knowledge, these are the most efficient green PeLEDs up to now. In addition, a threefold increase in the T50 operational time of the devices was observed, compared to control samples. These findings provide a simple and effective strategy to make highly efficient perovskite polycrystalline films and their optoelectronics devices.

7.
Small ; 16(50): e2005246, 2020 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-33230955

RESUMEN

Cesium lead iodide (CsPbI3 ) perovskite has gained great attention due to its potential thermal stability and appropriate bandgap (≈1.73 eV) for tandem cells. However, the moisture-induced thermodynamically unstable phase and large open-circuit voltage (VOC ) deficit and also the low efficiency seriously limit its further development. Herein, long chain phenylethylammonium (PEA) is utilized into CsPbI3 perovskite to stabilize the orthorhombic black perovskite phase (γ-CsPbI3 ) under ambient condition. Furthermore, the moderate lead acetate (Pb(OAc)2 ) is controlled to combine with phenylethylammonium iodide to form the 2D perovskite, which can dramatically suppress the charge recombination in CsPbI3 . Unprecedentedly, the resulted CsPbI3 solar cells achieve a 17% power conversion efficiency with a record VOC of 1.33 V, the VOC deficit is only 0.38 V, which is close to those in organic-inorganic perovskite solar cells (PSCs). Meanwhile, the PEA modified device maintains 94% of its initial efficiency after exceeding 2000 h of storage in the low-humidity controlled environment without encapsulation.

8.
Nat Commun ; 11(1): 4165, 2020 Aug 20.
Artículo en Inglés | MEDLINE | ID: mdl-32820166

RESUMEN

Perovskite light-emitting diodes (PeLEDs) have showed significant progress in recent years; the external quantum efficiency (EQE) of electroluminescence in green and red regions has exceeded 20%, but the efficiency in blue lags far behind. Here, a large cation CH3CH2NH2+ is added in PEA2(CsPbBr3)2PbBr4 perovskite to decrease the Pb-Br orbit coupling and increase the bandgap for blue emission. X-ray diffraction and nuclear magnetic resonance results confirmed that the EA has successfully replaced Cs+ cations to form PEA2(Cs1-xEAxPbBr3)2PbBr4. This method modulates the photoluminescence from the green region (508 nm) into blue (466 nm), and over 70% photoluminescence quantum yield in blue is obtained. In addition, the emission spectra is stable under light and thermal stress. With configuration of PeLEDs with 60% EABr, as high as 12.1% EQE of sky-blue electroluminescence located at 488 nm has been demonstrated, which will pave the way for the full color display for the PeLEDs.

9.
Adv Mater ; 31(49): e1905143, 2019 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-31631443

RESUMEN

Cesium-based inorganic perovskite solar cells (PSCs) are promising due to their potential for improving device stability. However, the power conversion efficiency of the inorganic PSCs is still low compared with the hybrid PSCs due to the large open-circuit voltage (VOC ) loss possibly caused by charge recombination. The use of an insulated shunt-blocking layer lithium fluoride on electron transport layer SnO2 for better energy level alignment with the conduction band minimum of the CsPbI3- x Brx and also for interface defect passivation is reported. In addition, by incorporating lead chloride in CsPbI3- x Brx precursor, the perovskite film crystallinity is significantly enhanced and the charge recombination in perovksite is suppressed. As a result, optimized CsPbI3- x Brx PSCs with a band gap of 1.77 eV exhibit excellent performance with the best VOC as high as 1.25 V and an efficiency of 18.64%. Meanwhile, a high photostability with a less than 6% efficiency drop is achieved for CsPbI3- x Brx PSCs under continuous 1 sun equivalent illumination over 1000 h.

10.
J Phys Chem Lett ; 10(11): 2892-2897, 2019 Jun 06.
Artículo en Inglés | MEDLINE | ID: mdl-31090418

RESUMEN

Quasi-two-dimensional (quasi-2D) perovskites are efficient luminescent materials due to their self-assembled quantum-well structure. We found that the organic cations have a significant effect on the structure and performance of quasi-2D perovskite-based light-emitting diodes (LEDs). Two classic organic cations, formamidinium (FA) and methylammonium (MA), were chosen for investigation. The MA-based quasi-2D perovskite has the largest band-gap n = 1 phase and a photoluminescence quantum yield (PLQY) as high as 85.3%, whereas this n = 1 phase is almost absent in the FA-based quasi-2D perovskite, which shows a moderate PLQY of 73.5%. However, the FA-based perovskite shows a much higher external quantum efficiency (15.4%) than the MA-based perovskite (0.93%) in LEDs. The lower electroluminescence efficiency of the MA-based perovskite could be ascribed to the poor hole injection. These results showed the importance of rational design of the quasi-2D perovskite for efficient LEDs.

11.
Nat Commun ; 9(1): 2225, 2018 06 08.
Artículo en Inglés | MEDLINE | ID: mdl-29884815

RESUMEN

Inorganic halide perovskites such as cesium lead halide are promising due to their excellent thermal stability. Cesium lead iodide (CsPbI3) has a bandgap of 1.73 eV and is very suitable for making efficient tandem solar cells, either with low-bandgap perovskite or silicon. However, the phase instability of CsPbI3 is hindering the further optimization of device performance. Here, we show that high quality and stable α-phase CsPbI3 film is obtained via solvent-controlled growth of the precursor film in a dry environment. A 15.7% power conversion efficiency of CsPbI3 solar cells is achieved, which is the highest efficiency reported for inorganic perovskite solar cells up to now. And more importantly, the devices can tolerate continuous light soaking for more than 500 h without efficiency drop.

12.
Nat Commun ; 9(1): 1169, 2018 03 16.
Artículo en Inglés | MEDLINE | ID: mdl-29549254

RESUMEN

The original version of this Article omitted an acknowledgement to the source of Fig. 1a. The following has been added to the end of the caption to Fig. 1: 'Figure 1a adapted from ref. 13 (copyright 2016 Macmillan Publishers)'. This has been corrected in the PDF and HTML versions of the Article.

13.
Nat Commun ; 9(1): 570, 2018 02 08.
Artículo en Inglés | MEDLINE | ID: mdl-29422600

RESUMEN

Perovskite light-emitting diodes (LEDs) are attracting great attention due to their efficient and narrow emission. Quasi-two-dimensional perovskites with Ruddlesden-Popper-type layered structures can enlarge exciton binding energy and confine charge carriers and are considered good candidate materials for efficient LEDs. However, these materials usually contain a mixture of phases and the phase impurity could cause low emission efficiency. In addition, converting three-dimensional into quasi-two-dimensional perovskite introduces more defects on the surface or at the grain boundaries due to the reduction of crystal sizes. Both factors limit the emission efficiency of LEDs. Here, firstly, through composition and phase engineering, optimal quasi-two-dimensional perovskites are selected. Secondly, surface passivation is carried out by coating organic small molecule trioctylphosphine oxide on the perovskite thin film surface. Accordingly, green LEDs based on quasi-two-dimensional perovskite reach a current efficiency of 62.4 cd A-1 and external quantum efficiency of 14.36%.

14.
Sci Bull (Beijing) ; 63(11): 726-731, 2018 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-36658822

RESUMEN

Perovskite crystal film quality is critical for obtaining efficient perovskite solar cells. Anti-solvent processing was used for fast crystallization of perovskite precursor film, which can form dense perovskite film. However, the crystals from this method are usually small due to the fast crystal growth process, which could lead to grain boundary recombination. Here, element chloride is introduced to enhance the perovskite layer crystallinity via slowing down the perovskite crystallization process by simultaneous introduction of methylammounium chloride (MACl) and cesium chloride (CsCl) into precursor solution. As a result, we achieve high quality of pin-hole free perovskite film with large crystal size. A power conversion efficiency of 21.55% with free of hysteresis of the device is obtained, which is among the highest efficiency of planar structure perovskite solar cells.

15.
Adv Mater ; 29(46)2017 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-29044741

RESUMEN

Low temperature solution processed planar-structure perovskite solar cells gain great attention recently, while their power conversions are still lower than that of high temperature mesoporous counterpart. Previous reports are mainly focused on perovskite morphology control and interface engineering to improve performance. Here, this study systematically investigates the effect of precise stoichiometry, especially the PbI2 contents on device performance including efficiency, hysteresis and stability. This study finds that a moderate residual of PbI2 can deliver stable and high efficiency of solar cells without hysteresis, while too much residual PbI2 will lead to serious hysteresis and poor transit stability. Solar cells with the efficiencies of 21.6% in small size (0.0737 cm2 ) and 20.1% in large size (1 cm2 ) with moderate residual PbI2 in perovskite layer are obtained. The certificated efficiency for small size shows the efficiency of 20.9%, which is the highest efficiency ever recorded in planar-structure perovskite solar cells, showing the planar-structure perovskite solar cells are very promising.

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