Colloidal Synthesis of Single-Layer Quasi-Ruddlesden–Popper Phase Bismuth-Based Two-Dimensional Perovskite Nanosheets with Controllable Optoelectronic Properties

Lee, Jacob T.; Seifert, Soenke; Sardar, Rajesh

doi:10.1021/acs.chemmater.1c00857

Title: Colloidal Synthesis of Single-Layer Quasi-Ruddlesden–Popper Phase Bismuth-Based Two-Dimensional Perovskite Nanosheets with Controllable Optoelectronic Properties

Journal Article · Tue Jul 20 00:00:00 EDT 2021 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.1c00857· OSTI ID:1833589

Lee, Jacob T. ^[1]; Seifert, Soenke ^[2];

^[3]

Indiana Univ.-Purdue Univ. Indianapolis (IUPUI), Indianapolis, IN (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Indiana Univ.-Purdue Univ. Indianapolis (IUPUI), Indianapolis, IN (United States); Indiana Univ.-Purdue Univ. Indianapolis (IUPUI), Indianapolis, IN (United States). Integrated Nanosystems Development Inst.

Single- and few-layered two-dimensional (2D) nanomaterials have attracted intense research interest in the last two decades due to their unique electronic and optoelectronic properties leading to various potential applications. Herein, we report the colloidal synthesis of Bi-based 2D perovskite nanosheets (PEG6-NH₃+)_nCs_3-nBi₂X₉, where X = CI, Br, and I, through careful design of reaction conditions and selection of poly(ethylene glycol) (PEG6) surface passivating ligands. The 2D nanosheets are similar to 5 nm in thickness with micron-sized lateral dimensions and display composition-dependent band gap and work function modulation. Furthermore, small-angle X-ray scattering analysis substantiates that the individual inorganic crystal layer, Cs_3-nBi₂X₉, is separated by the spacer, PEG6 ligand. Additionally, we determined that PEG6-NH₂ is an essential passivating ligand and spacer for the formation of Bi-based 2D nanosheets. Most importantly, controlled crystallization of the colloidal dispersion of nanosheets results in the formation of superlattice microstructures of the quasi-Ruddlesden-Popper phase. These microstructures can be exfoliated to ultrathin nanosheets by overcoming the van der Waals interaction between the organic passivating layers. The controlled synthesis of lead-free 2D perovskite nanosheets presented here can expand their utility to photocatalytic and optoelectronic applications with reduced toxicity.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC); National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357; DMR-1747582; ECCS-2025064

OSTI ID:: 1833589

Journal Information:: Chemistry of Materials, Vol. 33, Issue 15; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Lattices
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Title: Colloidal Synthesis of Single-Layer Quasi-Ruddlesden–Popper Phase Bismuth-Based Two-Dimensional Perovskite Nanosheets with Controllable Optoelectronic Properties

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