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Title: Structural Tunability and Diversity of Two‐Dimensional Lead Halide Benzenethiolate

Abstract

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, Pb 2 X(S‐C 6 H 5 ) 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 Pb 2 X(S‐C 6 H 5 ) 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.

Authors:
 [1];  [2];  [1];  [1];  [3];  [3];  [3];  [2]; ORCiD logo [1]
  1. Davidson School of Chemical Engineering Purdue University West Lafayette IN 47907 United States
  2. School of Materials Engineering Purdue University West Lafayette IN 47907 United States
  3. Department of Chemistry Purdue University West Lafayette IN 47907 United States
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1630224
Grant/Contract Number:  
SC0016356
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
Chemistry - A European Journal
Additional Journal Information:
Journal Name: Chemistry - A European Journal Journal Volume: 26 Journal Issue: 29; Journal ID: ISSN 0947-6539
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Coffey, Aidan H., Yoo, Pilsun, Kim, Dong Hee, Akriti,, Zeller, Matthias, Avetian, Sona, Huang, Libai, Liao, Peilin, and Dou, Letian. Structural Tunability and Diversity of Two‐Dimensional Lead Halide Benzenethiolate. Germany: N. p., 2020. Web. doi:10.1002/chem.201905790.
Coffey, Aidan H., Yoo, Pilsun, Kim, Dong Hee, Akriti,, Zeller, Matthias, Avetian, Sona, Huang, Libai, Liao, Peilin, & Dou, Letian. Structural Tunability and Diversity of Two‐Dimensional Lead Halide Benzenethiolate. Germany. https://doi.org/10.1002/chem.201905790
Coffey, Aidan H., Yoo, Pilsun, Kim, Dong Hee, Akriti,, Zeller, Matthias, Avetian, Sona, Huang, Libai, Liao, Peilin, and Dou, Letian. Thu . "Structural Tunability and Diversity of Two‐Dimensional Lead Halide Benzenethiolate". Germany. https://doi.org/10.1002/chem.201905790.
@article{osti_1630224,
title = {Structural Tunability and Diversity of Two‐Dimensional Lead Halide Benzenethiolate},
author = {Coffey, Aidan H. and Yoo, Pilsun and Kim, Dong Hee and Akriti, and Zeller, Matthias and Avetian, Sona and Huang, Libai and Liao, Peilin and Dou, Letian},
abstractNote = {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, Pb 2 X(S‐C 6 H 5 ) 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 Pb 2 X(S‐C 6 H 5 ) 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.},
doi = {10.1002/chem.201905790},
journal = {Chemistry - A European Journal},
number = 29,
volume = 26,
place = {Germany},
year = {Thu Mar 19 00:00:00 EDT 2020},
month = {Thu Mar 19 00:00:00 EDT 2020}
}

Journal Article:
Free Publicly Available Full Text
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https://doi.org/10.1002/chem.201905790

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