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

Worley, Chris; Yangui, Aymen; Roccanova, Rachel; Du, Mao‐Hua; Saparov, Bayrammurad

doi:10.1002/chem.201901112

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

Journal Article · Tue Jul 02 00:00:00 EDT 2019 · Chemistry - A European Journal

DOI:https://doi.org/10.1002/chem.201901112· OSTI ID:1545209

Worley, Chris ^[1];

^[1]; Roccanova, Rachel ^[1]; Du, Mao‐Hua ^[2];

^[1]

Univ. of Oklahoma, Norman, OK (United States). Dept. of Chemistry and Biochemistry
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division

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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1545209

Alternate ID(s):: OSTI ID: 1530632

Journal Information:: Chemistry - A European Journal, Vol. 25, Issue 42; ISSN 0947-6539

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 13 works

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Additive-assisted synthesis and optoelectronic properties of (CH ₃ NH ₃ ) ₄ Bi ₆ I ₂₂ Sharma, Manila; Yangui, Aymen; Lusson, Alain Inorganic Chemistry Frontiers, Vol. 7, Issue 7 https://doi.org/10.1039/c9qi01574d	journal	January 2020
Lead-Free Perovskites for Lighting and Lasing Applications: A Minireview Ushakova, Elena V.; Cherevkov, Sergei A.; Kuznetsova, Vera A. Materials, Vol. 12, Issue 23 https://doi.org/10.3390/ma12233845	journal	November 2019

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