Novel quantum-dot light-emitting diodes based on all-inorganic perovskite CsPbX3 (X = Cl, Br, I) nanocrystals are reported. The well-dispersed, single-crystal quantum dots (QDs) exhibit high quantum yields, and tunable light emission wavelength. The demonstration of these novel perovskite QDs opens a new avenue toward designing optoelectronic devices, such as displays, photodetectors, solar cells, and lasers.
Solution-processed CsPbBr quantum-dot light-emitting diodes with a 50-fold external quantum efficiency improvement (up to 6.27%) are achieved through balancing surface passivation and carrier injection via ligand density control (treating with hexane/ethyl acetate mixed solvent), which induces the coexistence of high levels of ink stability, photoluminescence quantum yields, thin-film uniformity, and carrier-injection efficiency.
Printed flexible photodetectors based on 2D inorganic perovskites with atomic thickness show excellent photosensing with fast rise and decay response times. As-synthesized nanosheets can easily be dispersed in various solvents, leading to large-area, crack-free, low-roughness, flexible films after printing. This study demonstrates that all-inorganic perovskite CsPbX3 nanosheets as a new class of 2D semiconductors have huge potential for flexible optoelectronic applications.
Highly efficient perovskite QLEDs can be realized when QD films possess two crucial synergistic parameters: highly luminescent features and effective electric transport properties. Regarding the emissive properties of QD films, although long organic ligands perfectly passivated the QD's surface and endowed ink with the near-unity luminescent properties with a PLQY approaching 100%, [11,12] the films generally exhibited a relatively low PLQY of about 40% due to the formation of nonradiative recombination centers. This phenomenon results from the dynamic characteristic of the bonding between the QD's surface and organic capping ligands, leading to the mismatched ligands during the film-forming process. [13,14] Meanwhile, these ligands act as electrically insulating layers on the QD's surface resulting in inefficient carrier injection and transportation, [15,16] which are detrimental to device performance. To enhance the electric properties of QD films, much attention [17,18] has been devoted to the development of ligand strategies that minimize the interparticle spacing. For example, Li et al. demonstrated an effective enhancement in electrical properties and EQE of CsPbBr 3 QLEDs through the control of surface ligand density. [9] Through ligand-exchange strategies, [8,19] a relatively short (C12) ligand, didodecyl dimethyl ammonium bromide (DDAB), was used to enhance device performance, obtaining an EQE of 8.73% under an effective washing process. Unfortunately, these methods are still based on long organic ligands, which cannot render the QD solid with ideal carrier injection and transportation features. Thus, it is significantly crucial to find an effective and feasible strategy to control the surface state of perovskite QDs, which could guarantee the high exciton recombination and carrier injection in constructing high-performance electroluminescent (EL) devices.Inorganic ligands with less space separation among particles could effectively enhance the electrical properties of QD films. [20,21] Meanwhile, they also improved the PL features through the reduce of the defect-related nonradiative recombination, which has been proven in traditional QDs. [22][23][24][25] For example, the halide-related ligands have improved the luminescent feature and radiative recombination in Cd-based QDs, which was realized by the ligand-exchange process. [20,26,27] But such a strategy is not feasible for perovskite QDs because they Perovskite quantum dots (QDs) with high photoluminescence quantum yields (PLQYs) and narrow emission peak hold promise for next-generation flexible and high-definition displays. However, perovskite QD films often suffer from low PLQYs due to the dynamic characteristics between the QD's surface and organic ligands and inefficient electrical transportation resulting from long hydrocarbon organic ligands as highly insulating barrier, which impair the ensuing device performance. Here, a general organic-inorganic hybrid ligand (OIHL) strategy is reported on to passivate perovskite QDs for highly efficient el...
Developing low-cost and high-quality quantum dots (QDs) or nanocrystals (NCs) and their corresponding efficient light-emitting diodes (LEDs) is crucial for the next-generation ultra-high-definition flexible displays. Here, there is a report on a room-temperature triple-ligand surface engineering strategy to play the synergistic role of short ligands of tetraoctylammonium bromide (TOAB), didodecyldimethylammonium bromide (DDAB), and octanoic acid (OTAc) toward "ideal" perovskite QDs with a high photoluminescence quantum yield (PLQY) of >90%, unity radiative decay in its intrinsic channel, stable ink characteristics, and effective charge injection and transportation in QD films, resulting in the highly efficient QD-based LEDs (QLEDs). Furthermore, the QD films with less nonradiative recombination centers exhibit improved PL properties with a PLQY of 61% through dopant engineering in A-site. The robustness of such properties is demonstrated by the fabrication of green electroluminescent LEDs based on CsPbBr QDs with the peak external quantum efficiency (EQE) of 11.6%, and the corresponding peak internal quantum efficiency (IQE) and power efficiency are 52.2% and 44.65 lm W , respectively, which are the most-efficient perovskite QLEDs with colloidal CsPbBr QDs as emitters up to now. These results demonstrate that the as-obtained QD inks have a wide range application in future high-definition QD displays and high-quality lightings.
All-inorganic perovskites have high carrier mobility, long carrier diffusion length, excellent visible light absorption, and well overlapping with localized surface plasmon resonance (LSPR) of noble metal nanocrystals (NCs). The high-performance photodetectors can be constructed by means of the intrinsic outstanding photoelectric properties, especially plasma coupling. Here, for the first time, inorganic perovskite photodetectors are demonstrated with synergetic effect of preferred-orientation film and plasmonic with both high performance and solution process virtues, evidenced by 238% plasmonic enhancement factor and 10 on/off ratio. The CsPbBr and Au NC inks are assembled into high-quality films by centrifugal-casting and spin-coating, respectively, which lead to the low cost and solution-processed photodetectors. The remarkable near-field enhancement effect induced by the coupling between Au LSPR and CsPbBr photogenerated carriers is revealed by finite-difference time-domain simulations. The photodetector exhibits a light on/off ratio of more than 10 under 532 nm laser illumination of 4.65 mW cm . The photocurrent increases from 0.67 to 2.77 μA with centrifugal-casting. Moreover, the photocurrent rises from 245.6 to 831.1 μA with Au NCs plasma enhancement, leading to an enhancement factor of 238%, which is the most optimal report among the LSPR-enhanced photodetectors, to the best of our knowledge. The results of this study suggest that all-inorganic perovskites are promising semiconductors for high-performance solution-processed photodetectors, which can be further enhanced by Au plasmonic effect, and hence have huge potentials in optical communication, safety monitoring, and biological sensing.
Visible‐infrared dual‐modal light harvesting is crucial for various optoelectronic devices, particularly for solar cells and photodetectors. For the first time, this study reports on large 25 cm3‐volume all‐inorganic perovskite CsPbBr3 single crystal (SC) with an emphasis on the observed visible‐infrared dual‐modal light harvesting and sensing as demonstrated by the high‐performance visible‐infrared dual‐modal photodetectors. First, ultralarge 25 cm3‐volume CsPbBr3 SC ingots with trapping state density as low as of 1 × 109 cm−3 have been achieved by a modified Bridgman growth method. The volume reported here is the largest CsPbX3 (X = Cl, Br, I) all‐inorganic perovskite system up to now, and the SC can be facilely cut into SC wafers with a diameter of 25 mm for various optoelectronic devices. Furthermore, these CsPbBr3 SCs exhibit a visible absorbance coefficient, a near‐infrared (IR) two‐phonon absorption coefficient, a carrier diffusion length, and a mobility as high as of 105 cm−1, 3.7 cm per Goeppert‐Mayer (GM), 10 µm and 2000 cm2 V−1 s−1, respectively. These merits match well to the requirements of high‐performance Vis‐IR dual‐modal light harvesting optoelectronic devices, which has been demonstrated by the CsPbBr3 SC photodetectors operated under the irradiation of both visible and IR light sources with light on/off ratio higher than 103. These results demonstrate the CsPbBr3 SCs with high visible‐infrared dual‐modal light harvesting capability and excellent electrical transporting properties have a huge potential in various optoelectronic devices, such as solar cells, photodetectors, and lasers.
Image sensor arrays are widely used in digital cameras, smartphones, and biorobots. However, most commercial image arrays rely on the dichroic prisms or a set of interference filters to distinguish characteristic color spectrum, which significantly increases the cost and fabrication processing complexity. In this work, an ultranarrow response photodetector with full-width at half-maximum being ∼12 nm and specific detectivity over 1011 Jones at 545 nm are successfully achieved in CsPbBr3 polycrystalline films using freeze-drying casting method to adjust the surface-charge recombination. To our best knowledge, this is the narrowest spectrum response for perovskite photodetectors in the visible light waveband. More importantly, a series of narrowband photodetectors are developed to enhance diverse selectivity for target signals covering from blue light to red light via bandgap tuning in CsPbX3 by tailoring the halide component. Finally, an integrated sensing array with CsPbX3 (X = Cl, Br, I) narrowband photodetectors acting as color recognition cones is constructed, which presents clear color and shape recognition paving the way for commercialization of perovskite photodetector in artificial vision.
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