Ligand Structure Directed Dimensionality Reduction (2D →1D) in Lead Bromide Perovskite

Bakthavatsalam, Rangarajan and Haris, Muhammed P U and Raavi, Sai Santosh Kumar (2019) Ligand Structure Directed Dimensionality Reduction (2D →1D) in Lead Bromide Perovskite. The Journal of Physical Chemistry C. ISSN 1932-7447

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Low dimensional (2D, 1D) lead halide perovskites are currently attracting huge research interest due to their enabling properties. Demonstrating synthetic control on the dimensionality/structure of these perovskites is highly challenging. Dimensionality in these perovskites is largely dictated by the nature/structure and composition of the incorporating ligands and the utilized synthetic conditions. Here, we demonstrate chemical composition based control on reduction of dimensionality (2D→1D) for lead bromide perovskite utilizing 2-(2-Aminoethyl)isothiourea dihydrobromide as a common precursor ligand (Isothio Bromide). Controlling the hydrothermal reaction parameters (temperature, time) at a fixed precursor ratio affords corner-shared, contorted 2D sheet perovskite and corner-shared, contorted, chiral 1D chain perovskite. Such dimensionality reduction leads to contrasting photo-physical properties: 1D chain perovskite shows long lived and self-trapped broad band emission whereas 2D perovskite shows short lived, band edge emission with long tail. Mechanistic studies and single crystal structure analysis reveal the incorporation of the utilized precursor ligand (Isothio Bromide) in 2D perovskite. Surprisingly, the 1D perovskite is found to be chiral (P21 space group) incorporating 2-(2-aminoethyldisulfanyl)ethanamine and ammonium ions as the achiral ligands generated in-situ due to hydrothermal cleavage of the precursor (Isothio Bromide) ligand. Such structural and compositional change of the ligands, that manifests different hydrogen bonding network in the resultant perovskite structure, plays a decisive role in dictating the final molecular formula and dimensionality/structure of the perovskite which largely controls their photo-physical properties.

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IITH Creators:
IITH CreatorsORCiD
Raavi, Sai Santosh Kumar
Item Type: Article
Subjects: Physics
Divisions: Department of Physics
Depositing User: Team Library
Date Deposited: 13 Jan 2020 05:46
Last Modified: 13 Jan 2020 05:46
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