Tautomeric mixture coordination enables efficient lead-free perovskite LEDs

Abstract

Lead-free perovskite light-emitting diodes (LEDs) prepared using tautomeric mixture coordination provide improved ordering in the crystal structure, reduced recombination and enhanced exciton binding energy compared with lead-containing perovskite-based LEDs. Lead halide perovskite light-emitting diodes (PeLEDs) have demonstrated remarkable optoelectronic performance^ 1 – 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_2SnI_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_2SnI_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 – 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.