RESUMEN
Quasi-2D perovskites are enchanting alternative materials for solar cells due to their intrinsic stability. The manipulation of crystal orientation of quasi-2D perovskites is indispensable to target efficient devices, however, the origin of orientation during the film fabrication process still lacks in-depth understanding and convincing evidence yet, which hinders further boosting the performance of photovoltaic devices. Herein, the crystallizing processes during spin-coating and annealing are probed by in situ grazing-incidence wide-angle X-ray scattering (GIWAXS), and the incident-angle-dependent GIWAXS is conducted to unveil the phase distribution in the films. It is found that undesirable lead iodide sol-gel formed intermediate phase would disturb oriented crystalline growth, resulting in random crystal orientation in poor quasi-2D films. A general strategy is developed via simple additive agent incorporation to suppress the formation of the intermediate phase. Accordingly, highly oriented perovskite films with reduced trap density and higher carrier mobility are obtained, which enables the demonstration of optimized quasi-2D perovskite solar cells with a power conversion efficiency of 15.2% as well as improved stability. This work paves a promising way to manipulate the quasi-2D perovskites nucleation and crystallization processes via tuning nucleation stage.
RESUMEN
Balanced charge injection is key to achieving perovskite light-emitting diodes (PeLEDs) with a low efficiency roll-off at a high brightness. The use of zinc oxide (ZnO) with a high electron mobility as the charge transport layers is desirable; however, photoluminescence (PL) quenching of a perovskite on ZnO always occurs. Here, a quasi-two-dimensional perovskite on ZnO is explored to uncover the PL quenching mechanism, mainly ascribed to the deprotonation of ammonium cations on the ZnO film in association with the decomposition of low-dimensional perovskite phases. Surprisingly, crystal plane-dependent PL quenching results indicate that the deprotonation rate strongly correlates with the crystal orientation of the ZnO surface. We developed a strategy for suppressing perovskite PL quenching by incorporating an atomic layer deposited Al2O3 onto the ZnO film. Consequently, an efficient inverted PeLED was achieved with a maximum external quantum efficiency of 17.7% and a less discernible efficiency roll-off at a high current density.
RESUMEN
Implementation of ammonium halides to trigger low-dimensional perovskite formation has been intensively investigated to achieve blue perovskite light-emitting diodes (PeLEDs). However, the general roles of the incorporated ammonium cations on the quality of the perovskite films, as well as device performance, are still unclear. It is indispensable to build a guideline to rationalize ammonium halides for decent blue emissive films. Here, by thoroughly investigating a series of ammonium cations containing the different number of ammonium groups and ionic radius, we reveal that the mechanism beyond the tunable emission wavelength, crystallization kinetics, and spectral stability of the obtained blue perovskite films is highly relevant to the molecular structure of the ammonium cations. In parallel with reducing the dimensionality to form normal Ruddlesden-Popper phases, the incorporated ammonium cations also likely modulate the Pb-Br orbit coupling through A-site engineering and generate either Dion-Jacobson or "hollow" perovskites, providing alternative routes to achieve efficient and stable blue emissive films. Our work paves a way to rationalize ammonium halides to develop prevailing active layers for further improving the performance of blue PeLEDs.
RESUMEN
Metal halide perovskite light-emitting diodes (PeLEDs) have been regarded as alternative candidates for full-color display applications with rapid progress to surge the external quantum efficiencies (EQEs) over 20%. However, in contrast to the high efficiencies of green, red, and near-infrared PeLEDs, the performance of their blue cousins is still lagging behind, especially the pure-blue one. Obtaining blue perovskite films with negligible nonradiative recombination loss and high stability is of great importance to realize efficient and spectrally stable blue PeLEDs. In this work, through partially replacing the toxic lead ions (Pb2+) with ecofriendly strontium ions (Sr2+) to tune the emission wavelength along with using passivation strategies, all-inorganic pure-blue perovskite films with a high photoluminescence quantum yield of 60.7% were achieved, which then delivered PeLEDs with a luminance of 510 cd m-2 and an EQE of 1.43%. The device yields a record radiance among the most efficient PeLEDs at 467 nm. In addition, the resultant PeLEDs displayed exceptional spectral stability during the electrical bias operation. Our work provides a promising avenue to develop environmentally friendly perovskite materials for efficient and spectrally stable pure-blue PeLEDs and beyond.