Matter
Volume 4, Issue 9, 1 September 2021, Pages 2936-2952
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Article
Colloidal synthesis and charge carrier dynamics of Cs4Cd1−xCuxSb2Cl12 (0 ≤ x ≤ 1) layered double perovskite nanocrystals

https://doi.org/10.1016/j.matt.2021.07.018Get rights and content
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Highlights

  • Colloidal Cs4CdSb2Cl12 LDP NCs are synthesized

  • Composition-structure-property relations are demonstrated using Cs4CdxCu1−xSb2Cl12 NCs

  • Cs4CdSb2Cl12 and Cs4CuSb2Cl12 LDP NCs show different charge carrier dynamics

  • Colloidal Cs4CdSb2Cl12 LDP NCs are solution processed into high-speed photodetectors

Progress and potential

Metal halide perovskite nanocrystals (NCs) have attracted tremendous attention due to their unique crystal structure and promising optoelectronic properties. Particularly, layered double perovskite (LDP) NCs with enriched compositional space and highly tunable properties are important for both fundamental studies and technological applications. Here, we report the colloidal synthesis of a series of Cs4Cd1−xCuxSb2Cl12 (0 ≤ x ≤ 1) LDP NCs with controlled metal compositions. Insights on the composition-structure-property relationships of the LDP NCs are explored through both material characterizations and theoretical calculations. Photogenerated charge carrier dynamics of the LDP NCs are investigated using ultrafast spectroscopic techniques. We show that such colloidal LDP NCs can be solution processed into a high-speed photodetector, demonstrating their potential in applications such as optical, photonic, and optoelectronic devices.

Summary

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 Cs4Cd1−xCuxSb2Cl12 (0 ≤ x ≤ 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.

Keywords

layered double perovskites
colloidal synthesis
nanocrystals
composition-structure-property relationship
compositional control
phase transition
charge carrier dynamics
photodetectors

Material advancement progression

MAP3: Understanding

Data and code availability

All data in the manuscript and supplemental information are available from the lead contact on request.

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