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Register a new userHighly efficient visible colloidal lead-halide perovskite nanocrystal light-emitting diodes
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Lead-halide perovskites have been attracting attention for potential use in solid-state lighting. Following the footsteps of solar cells, the field of perovskite light-emitting diodes (PeLEDs) has been growing rapidly. Their application prospects in lighting, however, remain still uncertain due to a variety of shortcomings in device performance including their limited levels of luminous efficiency achievable thus far. Here we show high-efficiency PeLEDs based on colloidal perovskite nanocrystals (PeNCs) synthesized at room temperature possessing dominant first-order excitonic radiation (enabling a photoluminescence quantum yield of 71% in solid film), unlike in the case of bulk perovskites with slow electron-hole bimolecular radiative recombination (a second-order process). In these PeLEDs, by reaching charge balance in the recombination zone, we find that the Auger nonradiative recombination, with its significant role in emission quenching, is effectively suppressed in low driving current density range. In consequence, these devices reach a record high maximum external quantum efficiency of 12.9% reported to date and an unprecedentedly high power efficiency of 30.3 lm W-1 at luminance levels above 1000 cd m-2 as required for various applications. These findings suggest that, with feasible levels of device performance, the PeNCs hold great promise for their use in LED lighting and displays.
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Solution-processed planar perovskite light-emitting diodes (LEDs) promise high-performance and cost-effective electroluminescent (EL) devices ideal for large-area display and lighting applications. Exploiting emission layers with high ratios of horizontal transition dipole moments (TDMs) is expected to boost photon outcoupling of planar LEDs. However, LEDs based on anisotropic perovskite nanoemitters remains to be inefficient (external quantum efficiency, EQE <5%), due to the difficulties of simultaneously controlling the orientations of TDMs, achieving high photoluminescence quantum yields (PLQYs) and realizing charge balance in the films of the assembled nanostructures. Here we demonstrate efficient EL from an in-situ grown continuous perovskite film comprising of a monolayer of face-on oriented nanoplatelets. The ratio of horizontal TDMs of the perovskite nanoplatelet films is ~84%, substantially higher than that of isotropic emitters (67%). The nanoplatelet film shows a high PLQY of ~75%. These merits enable LEDs with a peak EQE of 23.6%, representing the most efficient perovskite LEDs.
Perovskite-based optoelectronic devices have gained significant attention due to their remarkable performance and low processing cost, particularly for solar cells. However, for perovskite light-emitting diodes (LEDs), non-radiative charge carrier recombination has limited electroluminescence (EL) efficiency. Here we demonstrate perovskite-polymer bulk heterostructure LEDs exhibiting record-high external quantum efficiencies (EQEs) exceeding 20%, and an EL half-life of 46 hours under continuous operation. This performance is achieved with an emissive layer comprising quasi-2D and 3D perovskites and an insulating polymer. Transient optical spectroscopy reveals that photogenerated excitations at the quasi-2D perovskite component migrate to lower-energy sites within 1 ps. The dominant component of the photoluminescence (PL) is primarily bimolecular and is characteristic of the 3D regions. From PL quantum efficiency and transient kinetics of the emissive layer with/without charge-transport contacts, we find non-radiative recombination pathways to be effectively eliminated. Light outcoupling from planar LEDs, as used in OLED displays, generally limits EQE to 20-30%, and we model our reported EL efficiency of over 20% in the forward direction to indicate the internal quantum efficiency (IQE) to be close to 100%. Together with the low drive voltages needed to achieve useful photon fluxes (2-3 V for 0.1-1 mA/cm2), these results establish that perovskite-based LEDs have significant potential for light-emission applications.
Metal halide perovskites (MHPs) based phosphor-converted light-emitting diodes (pc-LEDs) are limited by the low MHP stability under storage/operation conditions. A few works have recently stablished the in-situ synthesis of MHPs into polymer matrices as an effective strategy to enhance MHPs stability with a low-cost fabrication. However, this is limited within petrochemical-based polymers. Herein, the first in-situ ambient preparation of highly luminescent and stable MHPs-bio-polymer filters (MAPbBr3 nanocrystals as emitter and poly(L-lactide acid) (PLLA) as matrix) with arbitrary areas (up to ca. 300 cm2) is reported. The MAPbBr3-PLLA phosphors feature a narrow emission (25 nm) with excellent photoluminescence quantum yields (more than 85%) and stabilities under ambient storage, water, and thermal stress. This is corroborated in green pc-LEDs featuring a low efficiency roll-off, excellent operational stability of ca. 600 h, and high luminous efficiencies of 65 lm W-1 that stand out the prior art (e.g., average lifetime of 200 h at 50 lm W-1). The filters are further exploited to fabricate white-emitting pc-LEDs with efficiencies of ca. 73 lm W-1 and x/y CIE color coordinates values of 0.33/0.32. Overall, this work stablishes a straightforward (one-pot/in-situ) and low-cost preparation (ambient/room temperature) of highly efficient and stable MHP-bio-polymer phosphors for highly performing and more sustainable lighting devices.
Excitonic/electronic coupling and cooperative interactions in self-assembled lead halide perovskite nanocrystals were reported to give rise to a collective low energy emission peak with accelerated dynamics. Here we report that similar spectroscopic features could appear as a result of the nanocrystal reactivity within the self-assembled superlattices. This is demonstrated by using CsPbBr3 nanocrystal superlattices under room temperature and cryogenic micro-photoluminescence spectroscopy. It is shown that keeping such structures under vacuum, a gradual contraction of the superlattices and subsequent coalescence of the nanocrystals occurs over several days. As a result, a narrow, low energy emission peak is observed at 4 K with a concomitant shortening of the photoluminescence lifetime due to the energy transfer between nanocrystals. When exposed to air, self-assembled CsPbBr3 nanocrystals develop bulk-like CsPbBr3 particles on top of the superlattices. At 4 K, these particles produce a distribution of narrow, low energy emission peaks with short lifetimes and excitation fluence-dependent, oscillatory decays, resembling the features of superfluorescence. Overall, the reactivity of CsPbBr3 nanocrystals dramatically alters the emission of their assemblies, which should not be overlooked when studying collective optoelectronic properties nor confused with superfluorescence effects.
This paper reviews recent progress in the synthesis of near-infrared (NIR) lead chalcogenide (PbX; PbX=PbS, PbSe, PbTe) quantum dots (QDs) and their applications in NIR QDs based light emitting diodes (NIR-QLEDs). It summarizes the strategies of how to synthesize high efficiency PbX QDs and how to realize high performance PbX based NIR-QLEDs.
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