Modulating Dimensionality of 2D Perovskite Layers for Efficient and Stable 2D/3D Perovskite Photodetectors.

Two-dimensional (2D) perovskites have been widely adopted for improving the performance and stability of three-dimensional (3D) metal halide perovskite devices. However, rational manipulation of the phase composition of 2D perovskites for suitable energy level alignment in 2D/3D perovskite photodetectors (PDs) has been rarely explored. Herein, we precisely controlled the dimensionality of the 2D perovskite on CsPbIBr films by tuning the polarity of the -butylammonium iodide (BAI)-based solvents. In comparison to the pure = 1 2D perovskite (ACN-BAI) formed by acetonitrile treatment, a mixture of = 1 and = 2 phases (IPA-BAI) generated by isopropanol (IPA) treatment guaranteed more robust defect passivation and favorable energy level alignment at the perovskite/hole transport layer interface. Consequently, the IPA-BAI PD exhibited a responsivity of 0.41 A W, a detectivity of 1.01 × 10 Jones, and a linear dynamic range of 120 dB. Furthermore, the mixed-phase 2D layer effectively shielded the 3D perovskite from moisture. The IPA-BAI device retained 76% of its initial responsivity after 500 h of nonencapsulated storage at 10% relative humidity. This research provides valuable insights into the dimensional modulation of 2D perovskites for further enhancing the performance of 2D/3D perovskite PDs.