Naphthalene Diimide Ammonium Directed Single-Crystalline Perovskites with “Atypical” Ambipolar Charge Transport Signatures in Two-Dimensional Limit

A single crystal of a lead–iodine-based 2D perovskite having naphthalene diimide ammonium (NDIA) molecules as organic layers was developed, and the charge transport property was studied using field-effect transistors (FETs) measurements. Structure determination reveals the layered alternative stacking of lead iodide sheets and NDIA bilayers. The presence of NDIA promoted the lead iodide octahedron to form the unique three-point co-planar [Pb3I10]4– unit, which then connected into the 2D network in a corner-sharing manner. The NDIA cations closely stacked into 1D chains within the bilayers that were being sandwiched between the inorganic layers. FET characteristics of the single crystal obtained at room temperature demonstrate VDS-dependent electron and hole transport behavior with mobilities reaching up to more than 5 × 10–3 cm2 V–1 s–1. The 1D stack of NDIAs contributes greatly to the performance improvement for both the charge transport and the stability