Murillo Henrique de Matos Rodrigues, Josiane A. Sobrinho, Arthur Pignataro Machado, Zeno C. Brandão, Ingrid D. Barcelos, Cilene Labre, Rodrigo Szostak, Ana F. Nogueira
High Resolution Image Download MS PowerPoint Slide Bulky 2D alkylammonium cations in metal halide perovskites offer a route to improve both structural stability and optoelectronic performance. This study systematically explores the incorporation of alkylammonium iodides with different chain lengths─dodecylammonium (C12), hexadecylammonium (C16), and octadecylammonium (C18)─into perovskite films for solar cells. Using spectroscopic and nanoscale characterization techniques, we show that C12 provides the best results: enhanced [111] orientation, reduced nonradiative recombination, uniform cation distribution, and improved vertical conductivity. Nanoscale X-ray diffraction and AFM-based infrared spectroscopy revealed that intermediate chain lengths enable favorable lattice expansion and interfacial passivation without hindering crystal growth. Solar cells based on C12-modified films reached power conversion efficiencies over 20%, surpassing both pristine and longer-chain formulations. These findings demonstrate that tuning alkyl chain length is an effective molecular design strategy to guide perovskite crystallization and improve device performance and stability.