Color Tuning for Perovskite Light-Emitting Diodes

Abstract: Metal halide perovskites (MHPs) are recognized as promising semiconductor materials for a variety of optical and electrical device applications due to their cost-effective and outstanding optoelectronic properties. As one of the most significant applications, perovskite light-emitting diodes (PeLEDs) hold promise for future lighting and display technologies, attributed to their high photoluminescence quantum yield (PLQY), high color purity, and tunable emission color. The emission colors of PeLEDs can be tuned by mixing the halide anions, adjusting the size of perovskite nanocrystals, or changing the dimensionality of perovskites. However, in practice, all these different approaches have their own advantages and challenges. This thesis centres around the color tunability of perovskites, aiming to develop PeLEDs with different colors using different approaches.We first demonstrate red and near-infrared PeLEDs using a straightforward approach – in situ solution-processed perovskite quantum dots (PQDs). PQDs prepared from colloidal approaches are widely reported and used in LEDs. In contrast, PQDs prepared from the in situ approaches are hardly reported, although they have advantages for device applications. By employing aromatic ammonium iodide (1-naphthylmethyl ammonium iodide, NMAI) as an agent into perovskite precursor solutions, together with annealing temperature modulation, we obtain in situ grown PQDs delivering high external quantum efficiencies (EQEs) of up to 11.0% with tunable electroluminescence (EL) spectra (667 - 790 nm). Our in situ generated PQDs based on pure-halogen perovskites can be easily obtained through a simple deposition process and free of phase segregation, making them a more promising approach for tuning the emission colors of perovskite LEDs.We then move to blue PeLEDs using cesium-based mixed-Br/Cl perovskites. Although mixed halides are a straightforward strategy to tune the emission color, PeLEDs based on this approach suffer from poor color stability, which is attributed to surface defects at grain boundaries. Under the condition of optical excitations, light density over a certain value (a threshold), oxygen, and surface defects at perovskite grain boundaries are found to be key factors inducing photoluminescence (PL) spectral instability of CsPb(Br1−xClx)3 perovskites. Upon electrical bias, defects at grain boundaries provide undesirable halide migration channels, responsible for EL spectral instability issues. Through effective defect passivation, the PL spectral resistance to oxygen is enhanced; moreover, high-performance and color-stable blue PeLEDs are achieved, delivering a maximum luminance of 5351 cd m–2 and a peak EQE of 4.55% with a peak emission wavelength at 489 nm. These findings provide new insights into the color instability issue of mixed halide blue perovskites, against which we also demonstrate an effective strategy.We finally realize single-emissive-layer (EML) white PeLEDs by employing a mixed halide perovskite film as the EML. In spite of high-performance monochromatic blue, green, and red colors, the development of white PeLEDs, especially for single-EML ones, remains a very big challenge. By effective modulation of the halide salt precursors, we achieve single-EML white PeLEDs with Commission Internationale de L’Eclairage (CIE) coordinates of (0.33, 0.33), close to those (0.3128, 0.3290) of the CIE standard illuminant D65. This work not only provides a successful demonstration of a single-EML white PeLED, but also provides useful guidelines for the future development of highperformance single-EML white PeLEDs.

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