Abstract

AbstractWe demonstrate that an ordered 2D perovskite can significantly boost the photoelectric performance of 2D/3D perovskite heterostructures. Using selective fluorination of phenyl‐ethyl ammonium (PEA) lead iodide to passivate 3D FA0.8Cs0.2PbI3, we find that the 2D/3D perovskite heterostructures passivated by a higher ordered 2D perovskite have lower Urbach energy, yielding a remarkable increase in photoluminescence (PL) intensity, PL lifetime, charge‐carrier mobilities (ϕμ), and carrier diffusion length (LD) for a certain 2D perovskite content. High performance with an ultralong PL lifetime of ≈1.3 μs, high ϕμ of ≈18.56 cm2 V−1 s−1, and long LD of ≈7.85 μm is achieved in the 2D/3D films when passivated by 16.67 % para‐fluoro‐PEA2PbI4. This carrier diffusion length is comparable to that of some perovskite single crystals (>5 μm). These findings provide key missing information on how the organic cations of 2D perovskites influence the performance of 2D/3D perovskite heterostructures.

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