Publication date: 15th December 2025
Scaling up perovskite light-emitting diodes (PeLEDs) remains challenging because interfacial quenching, charge imbalance, and efficiency roll-off become increasingly pronounced as device dimensions increase. Building on our previous work published in Nanoscale, where we first demonstrated the benefits of polymer-assisted interfacial engineering in nanocrystal-based emitters, this study advances that concept toward fully scalable architectures. We establish a comprehensive process–structure–performance framework for large-area PeLEDs by employing a thin polyvinylpyrrolidone (PVP) interlayer whose microstructure is stabilized through controlled vacuum conditioning. This combined strategy reduces interfacial quenching, enhances layer densification, and effectively removes residual solvents, thereby spatially decoupling the emissive nanocrystal layer from the hole-transport interface.
Through a systematic exploration of several processing parameters and device architectures, we demonstrate that PVP-assisted recombination-zone displacement and vacuum-driven solvent removal act synergistically to enhance charge balance and maintain stable emission at high brightness. Correlative analysis between deposition conditions, interlayer morphology, exciton dynamics, and electroluminescent behavior reveals clear trends: optimized interfacial passivation strengthens radiative recombination, suppresses non-radiative pathways, and significantly mitigates efficiency roll-off under elevated current densities. Moreover, stabilizing the polymer microstructure results in more uniform charge injection and delays the onset of degradation typically associated with larger pixels.
Overall, this work identifies vacuum-conditioned polymeric interlayers as a robust, generalizable strategy for enhancing the operational stability of solution-processed PeLEDs. Together with our previous findings [1], it provides a reproducible and scalable route toward high-efficiency perovskite emitters suitable for lighting and display applications.
The work of E. Ruby is supported by the project ANR CSUPER2. HAADF-STEM study was carried out within the MATMECA consortium, supported by the ANR-10-EQPX-37 contract, and has benefited from the facilities of the Laboratory MSSMat (UMR CNRS 8579), CentraleSupélec. The authors thank Arnaud BARTHELEMY for his assistance during Master 1 training and Dr. Bernard GEFFROY for his help with device characterization.
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