The crystal growth and orientation of two-dimensional (2D) perovskite films significantly impact solar cell performance. Here, we incorporated robust quadrupole-quadrupole interactions to govern the crystal growth of 2D Ruddlesden-Popper (RP) perovskites. This was achieved through the development of two unique semiconductor spacers, namely PTMA and 5FPTMA, with different dipole moments. The ((5FPTMA) (PTMA) ) MA Pb I (nominal n=5, 5F/PTMA-Pb) film shows a preferred vertical orientation, reduced grain boundaries, and released residual strain compared to (PTMA) MA Pb I (nominal n=5, PTMA-Pb), resulting in a decreased exciton binding energy and reduced electron-phonon coupling coefficients. In contrast to PTMA-Pb device with an efficiency of 15.66 %, the 5F/PTMA-Pb device achieved a champion efficiency of 18.56 %, making it among the best efficiency for 2D RP perovskite solar cells employing an MA-based semiconductor spacer. This work offers significant insights into comprehending the crystal growth process of 2D RP perovskite films through the utilization of quadrupole-quadrupole interactions between semiconductor spacers.
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