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Structural Tunability and Diversity of Two-Dimensional Lead Halide Benzenethiolate |
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| Authors: | Aidan H Coffey Pilsun Yoo Dong Hee Kim Akriti Dr Matthias Zeller Sona Avetian Prof Libai Huang Prof Peilin Liao Prof Letian Dou |
| Institution: | 1. Davidson School of Chemical Engineering, Purdue University, West Lafayette, IN, 47907 United States
These authors contributed equally to this work.;2. School of Materials Engineering, Purdue University, West Lafayette, IN, 47907 United States These authors contributed equally to this work.;3. Davidson School of Chemical Engineering, Purdue University, West Lafayette, IN, 47907 United States;4. Department of Chemistry, Purdue University, West Lafayette, IN, 47907 United States;5. School of Materials Engineering, Purdue University, West Lafayette, IN, 47907 United States |
| Abstract: | Two-dimensional (2D) organic-inorganic hybrid materials are currently of great interest for applications in electronics and optoelectronics. Here, the synthesis and optical properties of a new type of halide-organothiolate-mixed 2D hybrid material, Pb2X(S-C6H5)3, are reported, in which X is a halide (I, Br, or Cl). Different from conventional lead-based 2D layered materials, these compounds feature unusual five-coordinated lead centers with a stereochemically active electron lone pair on the lead atoms and four-coordinated iodine atoms. The Pb2X(S-C6H5)3 materials feature an indirect bandgap, strongly emissive long-lived self-trap states, and an extremely large Stokes shift. Interestingly, the optical bandgap of the materials can be tuned through variation of the halides; however, the photoluminescence is less sensitive to the composition and is more likely dominated by lead-sulfur lattice interactions or the lead lone-pair electrons. Our results support that a halide–organothiolate mixed anion hybrid structure offers a unique platform for discovering new exciting 2D electronic materials. |
| Keywords: | 2D materials electronic structures layered compounds lead halides S ligands |