Enhanced stability and linearly polarized emission from CsPbI3 perovskite nanoplatelets through A-site cation engineering

The anisotropy of perovskite nanoplatelets (PeNPLs) opens up many opportunities in optoelectronics, including enabling the emission of linearly polarized light. But the limited stability of PeNPLs is a pressing challenge, especially for red-emitting CsPbI₃. Herein, we address this limitation by alloying formamidinium (FA) into the perovskite cuboctahedral site. Unlike Cs/FA alloying in bulk thin films or nanocubes, FA incorporation in nanoplatelets requires meticulous control over the reaction conditions, given that nanoplatelets are obtained in kinetically-driven growth regimes instead of thermodynamically-driven conditions. Through in-situ photoluminescence (PL) measurements, we find that excess FA leads to uncontrolled growth, where phase impurities and nanoplatelets of multiple thicknesses co-exist. Restricting the FA content to up to 25% Cs substitution enables monodisperse PeNPLs, and increases the PL quantum yield, exciton lifetime, and stability in ambient air compared to CsPbI₃. The reduction in non-radiative recombination, improvement in the nanoplatelet aspect ratio, and higher ligand density lead to FA-containing PeNPLs more effectively forming edge-up superlattices, enhancing the PL degree of linear polarization from 5.1% (CsPbI₃) to 9.4% (Cs_0.75FA_0.25PbI₃). These fundamental insights show how the stability limitations of PeNPLs could be addressed, and these materials grown more precisely to improve their performance as polarized light emitters, critical for utilizing them in next-generation display, bioimaging, and communications applications.