Abstract

<h2>Summary</h2> The toxicity and instability of lead-based metal halide perovskites are the two main obstacles that prevent perovskite materials from implementation in applications. Recently, layered double perovskites (LDPs) have emerged as a new family of perovskite materials, which provide a new route to solve these problems by lead-component replacement and reduction of crystal structure dimensionality. However, LDP nanocrystals (NCs) have been rarely studied, limiting the further property exploration and application realization. Here, we report the colloidal synthesis of a series of Cs<sub>4</sub>Cd<sub>1−x</sub>Cu<sub>x</sub>Sb<sub>2</sub>Cl<sub>12</sub> (0 ≤ <i>x</i> ≤ 1) LDP NCs by tuning the stoichiometry of metal precursors. The composition-structure-property relationships of the resulting LDP NCs are studied through material characterizations, density functional theory calculations, and transient-absorption spectroscopy. In addition, we demonstrate that high-performance high-speed photodetectors can be fabricated using the colloidal LDP NCs through solution processing. This work premises further expansion of such LDP-based materials for both fundamental studies and application integrations.

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