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Register a new userHighly Efficient Blue Host-Free and Host-Guest Organic Light-Emitting Diodes Based on Carbene-Metal-Amides
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Carbene-metal-amide type photoemitters based on CF$_3$-substituted carbazolate ligands show sky-blue to deep-blue photoluminescence from charge-transfer excited states. They are suitable for incorporation into organic light-emitting diodes (OLEDs) by thermal vapour deposition techniques, either embedded within a high-triplet-energy host, or used host-free. We report high-efficiency OLEDs with emission ranging from yellow to blue (Commission Internationale de lEclairage (CIE) coordinates from [0.35, 0.53] to [0.17, 0.17]). The latter show a peak electroluminescence external quantum efficiency (EQE) of 20.9 $%$ in a polar host. We observe that the relative energies of CT and $^{3}$LE states influence the performance of deep-blue emission from carbene-metal-amide materials. We report prototype host-free blue devices with peak external quantum efficiency of 17.3 $%$, which maintain high performance at brightness levels of 100 cd m$^{-2}$.
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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.
Carbene-Metal-Amide light-emitting diodes have recently shown internal quantum efficiencies approaching 100%, and there has been substantial debate concerning the cause of their exceptionally high efficiency. Here we present a theoretical description of CMAs, showing how a simple three-atom model can predict the form of the HOMO and LUMO, determine the polarization of transitions and the feasibility of spin-orbit coupling, as well as the qualitative dependence of excited state energies and oscillator strength on the twist angle. These results clarify many of the claims concerning CMAs and pave the way for the design of more efficient devices.
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.
The radiative recombination of injected charge carriers gives rise to electroluminescence (EL), a central process for light-emitting diode (LED) operation. It is often presumed in some emerging fields of optoelectronics, including perovskite and organic LEDs, that the minimum voltage required for light emission is the semiconductor bandgap divided by the elementary charge. Here we show for many classes of LEDs, including those based on metal halide perovskite, organic, chalcogenide quantum-dot and commercial III-V semiconductors, photon emission can be generally observed at record-low driving voltages of 36%-60% of their bandgaps, corresponding to a large apparent energy gain of 0.6-1.4 eV per emitted photon. Importantly, for various classes of LEDs with very different modes of charge injection and recombination (dark saturation current densities ranging from ~10^-35 to ~10^-21 mA/cm2), their EL intensity-voltage curves under low voltages exhibit similar behaviors, revealing a universal origin of ultralow-voltage device operation. Finally, we demonstrate as a proof-of-concept that perovskite LEDs can transmit data efficiently to a silicon detector at 1V, a voltage below the silicon bandgap. Our work provides a fresh insight into the operational limits of electroluminescent diodes, highlighting the significant potential of integrating low-voltage LEDs with silicon electronics for next-generation communications and computational applications.
The magnetoelectroluminescence of conjugated organic polymer films is widely accepted to arise from a polaron pair mechanism, but their magnetoconductance is less well understood. Here we derive a new relationship between the experimentally measurable magnetoelectroluminescence and magnetoconductance and the theoretically calculable singlet yield of the polaron pair recombination reaction. This relationship is expected to be valid regardless of the mechanism of the magnetoconductance, provided the mobilities of the free polarons are independent of the applied magnetic field (i.e., provided one discounts the possibility of spin-dependent transport). We also discuss the semiclassical calculation of the singlet yield of the polaron pair recombination reaction for materials such as poly(2,5-dioctyloxy-paraphenylene vinylene) (DOO-PPV), the hyperfine fields in the polarons of which can be extracted from light-induced electron spin resonance measurements. The resulting theory is shown to give good agreement with experimental data for both normal (H-) and deuterated (D-) DOO-PPV over a wide range of magnetic field strengths once singlet-triplet dephasing is taken into account. Without this effect, which has not been included in any previous simulation of magnetoelectroluminescence, it is not possible to reproduce the experimental data for both isotopologues in a consistent fashion. Our results also indicate that the magnetoconductance of DOO-PPV cannot be solely due to the effect of the magnetic field on the dissociation of polaron pairs.
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