Lead-Free Cs4CuSb2Cl12 Layered Double Perovskite Nanocrystals
- 7 July 2020
- journal article
- research article
- Published by American Chemical Society (ACS) in Journal of the American Chemical Society
- Vol. 142 (27), 11927-11936
- https://doi.org/10.1021/jacs.0c04919
Abstract
Concerns about the toxicity of lead-based perovskites have aroused great interest for the development of alternative lead-free perovskite-type materials. Recently, theoretical calculations predict that Pb2+ cations can be substituted by a combination of Cu2+ and Sb2+ cations to form a vacancy-ordered layered double perovskite structure with superior optoelectronic properties. However, accessibilities to this class of perovskite-type materials remain inadequate, hindering their practical implementations in various applications. Here, we report the first colloidal synthesis of Cs(4)CuSb(2)Cl(12 )perovskite-type nanocrystals (NCs). The resulting NCs exhibit a layered double perovskite structure with ordered vacancies and a direct band gap of 1.79 eV. A composition-structure-property relationship has been established by investigating a series of Cs(4)Cu(x)Ag(2-2x)Sb(2)Cl(12 )perovskite-type NCs (0 <= x <= 1). The composition induced crystal structure transformation, and thus, the electronic band gap evolution has been explored by experimental observations and further confirmed by theoretical calculations. Taking advantage of both the unique electronic structure and solution processability, we demonstrate that the Cs4CuSb2Cl12 NCs can be solution-processed as high-speed photodetectors with ultrafast photoresponse and narrow bandwidth. We anticipate that our study will prompt future research to design and fabricate novel and high-performance lead-free perovskite-type NCs for a range of applications.Funding Information
- Brown University
- U.S. Department of Education (P200A150037)
- U.S. Department of Energy (DE-AC02-06CH11357, DE-SC0012704)
This publication has 72 references indexed in Scilit:
- Quantum-Dot-Induced Cesium-Rich Surface Imparts Enhanced Stability to Formamidinium Lead Iodide Perovskite Solar CellsACS Energy Letters, 2019
- 14.1% CsPbI3 Perovskite Quantum Dot Solar Cells via Cesium Cation PassivationAdvanced Energy Materials, 2019
- Fusing Nanowires into Thin Films: Fabrication of Graded‐Heterojunction Perovskite Solar Cells with Enhanced PerformanceAdvanced Energy Materials, 2019
- Building bridges between halide perovskite nanocrystals and thin-film solar cellsSustainable Energy & Fuels, 2018
- Efficient Light-Emitting Diodes Based on in Situ Fabricated FAPbBr3 Nanocrystals: The Enhancing Role of the Ligand-Assisted Reprecipitation ProcessACS Nano, 2018
- Composition‐Graded Cesium Lead Halide Perovskite Nanowires with Tunable Dual‐Color Lasing PerformanceAdvanced Materials, 2018
- Genesis, challenges and opportunities for colloidal lead halide perovskite nanocrystalsNature Materials, 2018
- Quantum dot–induced phase stabilization of α-CsPbI 3 perovskite for high-efficiency photovoltaicsScience, 2016
- Quantum Dot Light‐Emitting Diodes Based on Inorganic Perovskite Cesium Lead Halides (CsPbX3)Advanced Materials, 2015
- Lead halide perovskite nanowire lasers with low lasing thresholds and high quality factorsNature Materials, 2015