Boosting Charge Transport in a 2D/3D Perovskite Heterostructure by Selecting an Ordered 2D Perovskite as the Passivator

Abstract

We 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 FA_0.8 Cs_0.2 PbI₃ , 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 (L_D ) 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 L_D of ≈7.85 μm is achieved in the 2D/3D films when passivated by 16.67 % para-fluoro-PEA₂ PbI₄ . 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.

Keywords: 2D/3D Heterostructures; Relative Structural Ordering; Structure-Property Relationship; Sum Frequency Generation.