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Tautomeric mixture coordination enables efficient lead-free perovskite LEDs

NATURE [2023]
Han Dongyuan, Wang Jie, Agosta Lorenzo, Zang Ziang, Zhao Bin, Kong Lingmei, Lu Haizhou, Mosquera-Lois Irea, Carnevali Virginia, Dong Jianchao, Zhou Jianheng, Ji Huiyu, Pfeifer Lukas, Zakeeruddin Shaik M., Yang Yingguo, Wu Bo, Rothlisberger Ursula, Yang Xuyong, Grätzel Michael, Wang Ning
ABSTRACT

Lead halide perovskite light-emitting diodes (PeLEDs) have demonstrated remarkable optoelectronic performance 1 , 2 , 3 . However, there are potential toxicity issues with lead 4 , 5 and removing lead from the best-performing PeLEDs—without compromising their high external quantum efficiencies—remains a challenge. Here we report a tautomeric-mixture-coordination-induced electron localization strategy to stabilize the lead-free tin perovskite TEA 2 SnI 4 (TEAI is 2-thiopheneethylammonium iodide) by incorporating cyanuric acid. We demonstrate that a crucial function of the coordination is to amplify the electronic effects, even for those Sn atoms that aren’t strongly bonded with cyanuric acid owing to the formation of hydrogen-bonded tautomeric dimer and trimer superstructures on the perovskite surface. This electron localization weakens adverse effects from Anderson localization and improves ordering in the crystal structure of TEA 2 SnI 4 . These factors result in a two-orders-of-magnitude reduction in the non-radiative recombination capture coefficient and an approximately twofold enhancement in the exciton binding energy. Our lead-free PeLED has an external quantum efficiency of up to 20.29%, representing a performance comparable to that of state-of-the-art lead-containing PeLEDs 6 , 7 , 8 , 9 , 10 , 11 , 12 . We anticipate that these findings will provide insights into the stabilization of Sn(II) perovskites and further the development of lead-free perovskite applications.

MATERIALS

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