Abstract
Inexpensive perovskite light-emitting devices fabricated by a simple wet chemical approach have recently demonstrated very prospective characteristics such as narrowband emission, low turn-on bias, high brightness, and high external quantum efficiency of electroluminescence, and have presented a good alternative to well-established technology of epitaxially grown III-V semiconducting alloys. Engineering of highly efficient perovskite light-emitting devices emitting green, red, and near-infrared light has been demonstrated in numerous reports and has faced no major fundamental limitations. On the contrary, the devices emitting blue light, in particular, based on 3D mixed-halide perovskites, suffer from electric field-induced phase separation (segregation). This crystal lattice defect-mediated phenomenon results in an undesirable color change of electroluminescence. Here we report a novel approach towards the suppression of the segregation in single-layer perovskite light-emitting electrochemical cells. Co-crystallization of direct band gap CsPb(Cl,Br) and indirect band gap CsPb(Cl,Br) phases in the presence of poly(ethylene oxide) during a thin film deposition affords passivation of surface defect states and an increase in the density of photoexcited charge carriers in CsPb(Cl,Br) grains. Furthermore, the hexahalide phase prevents the dissociation of the emissive grains in the strong electric field during the device operation. Entirely resistant to 5.7 × 10 V·m electric field-driven segregation light-emitting electrochemical cell exhibits stable emission at wavelength 479 nm with maximum external quantum efficiency 0.7%, maximum brightness 47 cd·m, and turn-on bias of 2.5 V.
Highlights
Over the past few years, all-inorganic lead halide perovskites have gained much attention from the scientific community [1,2,3,4]
The segregation dynamics in multilayer perovskite light-emitting devices (PeLEDs) [16,28] is remarkably affected by strong electric field of 1 × 106–107 V·m−1 decomposing the ionic lattice of perovskite and producing numerous defect states, and halide vacancies in particular. This drawback should be much more pronounced in single-layer perovskite light-emitting electrochemical cells (PeLECs) with a p-i-n junction created via dissociation of perovskite into negatively and positively charged species [29,30]. From this point of view, single-layer PeLECs based on CsPb(Cl,Br)3 compositions should operate at extreme conditions favorable for electric field-driven segregation, whereas development of the approaches to stabilize their blue color electroluminescence would allow these materials to compete with low-dimensional monohalide counterparts [16,18,19,20,31,32,33]
We report an original solvent engineering method for the fabrication of stabilized blue PeLECs with a single layer derived from a mixture of poly(ethylene oxide) (PEO) and CsCl:PbBr2 taken in various stoichiometric ratios (1:1, 5:4, 4:3)
Summary
Over the past few years, all-inorganic lead halide perovskites have gained much attention from the scientific community [1,2,3,4]. The segregation dynamics in multilayer PeLEDs [16,28] is remarkably affected by strong electric field of 1 × 106–107 V·m−1 decomposing the ionic lattice of perovskite and producing numerous defect states, and halide vacancies in particular This drawback should be much more pronounced in single-layer perovskite light-emitting electrochemical cells (PeLECs) with a p-i-n junction created via dissociation of perovskite into negatively and positively charged species [29,30]. From this point of view, single-layer PeLECs based on CsPb(Cl,Br) compositions should operate at extreme conditions favorable for electric field-driven segregation, whereas development of the approaches to stabilize their blue color electroluminescence would allow these materials to compete with low-dimensional monohalide counterparts [16,18,19,20,31,32,33].
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