Journal
INORGANIC CHEMISTRY
Volume 60, Issue 19, Pages 14629-14635Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.1c01669
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Funding
- National Natural Science Foundation of China [51532010, 51872028, 51832010]
- Fundamental Research Funds for the Central Universities [FRF-IDRY-19-005]
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The study reports the synthesis of three new Pb-free hybrid-layered-double perovskites and analyzes their optoelectronic properties, providing a new approach for the development of this type of semiconductor materials.
The Pb-free hybrid-layered-double perovskites (HLDPs) have been proposed as green and stable semiconducting materials for optoelectronic devices, but the synthesized members are still limited. Here, we report the synthesis of three new HLDPs, (C8H20N2)(2)AgMBr8 (M = In, Sb, and Bi), by a solution method using 1,4-bis(ammoniomethyl)cyclohexane (C8H20N22+) as the organic spacing cation. All three of these HLDPs show < 100 >-oriented layered structures with Ag and In/Sb/Bi order arranged in corner-sharing octahedral layers. The first-principle calculations indicate the indirect-gap nature of (C8H20N2)(2)AgInBr8 and (C8H20N2)(2)AgSbBr8, while their Bi counterpart shows a direct band gap after considering spin-orbit coupling. The band gaps obtained by diffuse-reflectance spectroscopy are 3.11, 2.60, and 2.70 eV for M = In, Sb, and Bi, respectively. (C8H20N2)(2)AgInBr8 shows a broadband red emission centered at 690 nm, and it is mainly attributed to the self-trapped-excitons mechanism. Our results not only provide a series of new Pb-free HLDPs with chemical diversity but also help us to further understand the structure-property relationships of HLDP materials.
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