The surface passivating and defect suppressing nature of Cd dopants and DDAB ligands in PNCs provides remarkable photoluminescence quantum yield and emission stability, leading to enhanced device efficiencies in blue PeLEDs.

Semiconducting lead halide perovskite nanocrystals (PNCs) are regarded as promising candidates for next‐generation optoelectronic devices due to their solution processability and outstanding optoelectronic properties. While the field of light‐emitting diodes (LEDs) and photovoltaics (PVs), two prime examples of optoelectronic devices, has recently seen a multitude of efforts toward high‐performance PNC‐based devices, realizing both devices with high efficiencies and stabilities through a single PNC processing strategy has remained a challenge.  In this work, diphenylpropylammonium (DPAI) surface ligands, found through a judicious ab‐initio‐based ligand search, are shown to provide a solution to this problem. The universal PNC ink with DPAI ligands presented here, prepared through a solution‐phase ligand‐exchange process, simultaneously allows single‐step processed LED and PV devices with peak electroluminescence external quantum efficiency of 17.00% and power conversion efficiency of 14.92% (stabilized output 14.00%), respectively. It is revealed that a careful design of the aromatic rings such as in DPAI is the decisive factor in bestowing such high performances, ease of solution processing, and improved phase stability up to 120 days. This work illustrates the power of ligand design in producing PNC ink formulations for high‐throughput production of optoelectronic devices; it also paves a path for “dual‐mode” devices with both PV and LED functionalities.

A polymer/small-molecule binary-blend hole transport layer provided balanced charge transport and efficient recombination of electrons and holes in the perovskite layer, and an optimal device based on the blended HTL shows the highest EQE of 5.30%.

Among the solution-processed devices, perovskite solar cells (PSCs) exhibit the highest power conversion efficiency (PCE) of over 25%; tremendous efforts are being undertaken to improve their stability. Recently, all-inorganic CsPbI2Br-based PSCs were reported to exhibit a significantly improved device stability, with a promising PCE of up to 16.79%. In this study, we report stable all-inorganic PSCs by incorporating novel dopant-free hole-transporting materials (HTMs). The synthesis strategy of the newly synthesized polymeric HTMs was similar to that of 2,2′,7,7′-tetrakis­(N,N-di-p-methoxyphenylamine)-9,9′-spirobifluorene (spiro-OMeTAD), with the exception that they were designed to exhibit dopant-free characteristics. In particular, their polymeric backbone structure was significantly simpler than that of spiro-OMeTADs, and they were easily synthesized in two steps from commercially available chemicals, with an overall yield of ∼50%. The cost of synthesis at the laboratory scale was calculated to be at least 2.4 times cheaper than that of spiro-OMeTADs. The PCE of dopant-free HTM-based PSCs was 11.01%, which is 1.5 times higher than that of the dopant-free spiro-OMeTAD-based devices (7.52%) and comparable to that of the doped spiro-OMeTAD-based devices (12.22%). Notably, the stability of the device based on our dopant-free HTM to atmospheric oxygen and moisture as well as heat and light irradiation was superior to that of devices based on doped and dopant-free spiro-OMeTAD HTMs. On consideration of the synthesis cost, device efficiency, and device stability, our dopant-free HTM is highly promising for all-inorganic PSCs.

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