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Title: (CH3NH3) AuX4·H2O (X=Cl, Br) and (CH3NH3) AuCl4: Low-Band Gap Lead-Free Layered Gold Halide Perovskite Materials

Abstract

Perovskite solar cells have recently enabled power conversion efficiency comparable to established technologies such as silicon and cadmium telluride. Ongoing efforts to improve the stability of halide perovskites in ambient air has yielded promising results. However, the presence of toxic heavy element lead (Pb) remains a major concern requiring further attention. Herein, we report three new Pb-free hybrid organic–inorganic perovskite-type halides based on gold (Au), (CH3NH3)AuBr4·H2O (1), (CH3NH3)AuCl4·H2O (2), and (CH3NH3)AuCl4 (3). Hydrated compounds 1 and 2 crystallize in a brand-new structure type featuring perovskite-derived 2D layers and 1D chains based on pseudo-octahedral AuX6 building blocks. In contrast, the novel crystal structure of the solvent-free compound 3 shows an exotic non-perovskite quasi-2D layered structure containing edge- and corner-shared AuCl6 octahedra. The use of Au metal instead of Pb results in unprecedented low band gaps below 2.5 eV for single-layered metal chlorides and bromides. Moreover, at room temperature the three compounds show a weak blue emission due to the electronic transition between Au-6s and Au-5d, in agreement with the density function theory (DFT) calculation results. These findings are discussed in the context of viability of Au-based halides as alternatives for Pb-based halides for optoelectronic applications.

Authors:
 [1]; ORCiD logo [1];  [1];  [2]; ORCiD logo [1]
  1. Univ. of Oklahoma, Norman, OK (United States). Dept. of Chemistry and Biochemistry
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1545209
Alternate Identifier(s):
OSTI ID: 1530632
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry - A European Journal
Additional Journal Information:
Journal Volume: 25; Journal Issue: 42; Journal ID: ISSN 0947-6539
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 13 HYDRO ENERGY; 30 DIRECT ENERGY CONVERSION; density functional calculations; diffuse reflectance; halides; low-band gap; perovskite phases

Citation Formats

Worley, Chris, Yangui, Aymen, Roccanova, Rachel, Du, Mao‐Hua, and Saparov, Bayrammurad. (CH3NH3) AuX4·H2O (X=Cl, Br) and (CH3NH3) AuCl4: Low-Band Gap Lead-Free Layered Gold Halide Perovskite Materials. United States: N. p., 2019. Web. https://doi.org/10.1002/chem.201901112.
Worley, Chris, Yangui, Aymen, Roccanova, Rachel, Du, Mao‐Hua, & Saparov, Bayrammurad. (CH3NH3) AuX4·H2O (X=Cl, Br) and (CH3NH3) AuCl4: Low-Band Gap Lead-Free Layered Gold Halide Perovskite Materials. United States. https://doi.org/10.1002/chem.201901112
Worley, Chris, Yangui, Aymen, Roccanova, Rachel, Du, Mao‐Hua, and Saparov, Bayrammurad. Tue . "(CH3NH3) AuX4·H2O (X=Cl, Br) and (CH3NH3) AuCl4: Low-Band Gap Lead-Free Layered Gold Halide Perovskite Materials". United States. https://doi.org/10.1002/chem.201901112. https://www.osti.gov/servlets/purl/1545209.
@article{osti_1545209,
title = {(CH3NH3) AuX4·H2O (X=Cl, Br) and (CH3NH3) AuCl4: Low-Band Gap Lead-Free Layered Gold Halide Perovskite Materials},
author = {Worley, Chris and Yangui, Aymen and Roccanova, Rachel and Du, Mao‐Hua and Saparov, Bayrammurad},
abstractNote = {Perovskite solar cells have recently enabled power conversion efficiency comparable to established technologies such as silicon and cadmium telluride. Ongoing efforts to improve the stability of halide perovskites in ambient air has yielded promising results. However, the presence of toxic heavy element lead (Pb) remains a major concern requiring further attention. Herein, we report three new Pb-free hybrid organic–inorganic perovskite-type halides based on gold (Au), (CH3NH3)AuBr4·H2O (1), (CH3NH3)AuCl4·H2O (2), and (CH3NH3)AuCl4 (3). Hydrated compounds 1 and 2 crystallize in a brand-new structure type featuring perovskite-derived 2D layers and 1D chains based on pseudo-octahedral AuX6 building blocks. In contrast, the novel crystal structure of the solvent-free compound 3 shows an exotic non-perovskite quasi-2D layered structure containing edge- and corner-shared AuCl6 octahedra. The use of Au metal instead of Pb results in unprecedented low band gaps below 2.5 eV for single-layered metal chlorides and bromides. Moreover, at room temperature the three compounds show a weak blue emission due to the electronic transition between Au-6s and Au-5d, in agreement with the density function theory (DFT) calculation results. These findings are discussed in the context of viability of Au-based halides as alternatives for Pb-based halides for optoelectronic applications.},
doi = {10.1002/chem.201901112},
journal = {Chemistry - A European Journal},
number = 42,
volume = 25,
place = {United States},
year = {2019},
month = {7}
}

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