Tautomeric mixture coordination enables efficient lead-free perovskite LEDs

Dongyuan Han, Jie Wang, Lorenzo Agosta, Ziang Zang, Bin Zhao, Lingmei Kong, Haizhou Lu (), Irea Mosquera-Lois, Virginia Carnevali, Jianchao Dong, Jianheng Zhou, Huiyu Ji, Lukas Pfeifer, Shaik M. Zakeeruddin, Yingguo Yang, Bo Wu, Ursula Rothlisberger, Xuyong Yang (), Michael Grätzel () and Ning Wang ()
Additional contact information
Dongyuan Han: Jilin University
Jie Wang: Jilin University
Lorenzo Agosta: École Polytechnique Fédérale de Lausanne (EPFL)
Ziang Zang: Jilin University
Bin Zhao: Jilin University
Lingmei Kong: Shanghai University
Haizhou Lu: École Polytechnique Fédérale de Lausanne (EPFL)
Irea Mosquera-Lois: École Polytechnique Fédérale de Lausanne (EPFL)
Virginia Carnevali: École Polytechnique Fédérale de Lausanne (EPFL)
Jianchao Dong: Jilin University
Jianheng Zhou: Jilin University
Huiyu Ji: Jilin University
Lukas Pfeifer: École Polytechnique Fédérale de Lausanne (EPFL)
Shaik M. Zakeeruddin: École Polytechnique Fédérale de Lausanne (EPFL)
Yingguo Yang: Chinese Academy of Sciences
Bo Wu: South China Normal University
Ursula Rothlisberger: École Polytechnique Fédérale de Lausanne (EPFL)
Xuyong Yang: Shanghai University
Michael Grätzel: École Polytechnique Fédérale de Lausanne (EPFL)
Ning Wang: Jilin University

Nature, 2023, vol. 622, issue 7983, 493-498

Abstract: Abstract Lead halide perovskite light-emitting diodes (PeLEDs) have demonstrated remarkable optoelectronic performance1–3. However, there are potential toxicity issues with lead4,5 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 TEA2SnI4 (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 TEA2SnI4. 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 PeLEDs6–12. We anticipate that these findings will provide insights into the stabilization of Sn(II) perovskites and further the development of lead-free perovskite applications.

Date: 2023
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DOI: 10.1038/s41586-023-06514-6

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