Modulating Quantum Well Width of Ferroelectric Ruddlesden–Popper Perovskites for Flexible Light Communication Device

Abstract 2D Ruddlesden–Popper perovskites exhibit significant ferroelectricity due to the spontaneous polarization of organic molecules. By modulating the quantum well width in 2D Ruddlesden–Popper perovskites BA₂MA_n‐1Pb_nBr_3n+1, a series of perovskites are adopted to realize adjustable polarization intensity and bandgap width. It is found that when n = 3, perovskite has the maximum polarization strength and optimal optoelectronic performance. In addition, flexible photodetectors with high mechanical stability are successfully fabricated based on n = 3 perovskite microplates. The fabricated flexible photodetectors exhibit high responsivity of 920 mA W⁻¹ and detectivity of 1.02 × 10¹¹ Jones, along with excellent flexibility and stability. After 3000 bending cycles, the photocurrent of n = 3 perovskites photodetector remains 81.8% of initial state. Besides, the photocurrent of n = 3 perovskites increase by 33 and 34 times after polarization at 0 and 3 V, respectively. And n = 3 perovskites exhibit a high polarization sensitivity with a current ratio of 2.09. On the basis of controllable regulation of the photocurrent through polarization, the application of flexible decoding optoelectronic devices by utilizing the correspondence between optical signals before and after polarization and binaries is achieved. These findings highlight the potential of modulating quantum well width in 2D Ruddlesden–Popper perovskites as a promising strategy for designing next‐generation flexible optoelectronic devices.