Vapor Growth of All-Inorganic 2D Ruddlesden–Popper Lead- and Tin-Based Perovskites

The 2D Ruddlesden-Popper (RP) perovskites Cs<sub>2</sub>PbI<sub>2</sub>Cl<sub>2</sub> (Pb-based, <i>n</i> = 1) and Cs<sub>2</sub>SnI<sub>2</sub>Cl<sub>2</sub> (Sn-based, <i>n</i> = 1) stand out as unique and rare instances of entirely inorganic constituents within the more expansive category of organic/inorganic 2D perovskites. These materials have recently garnered significant attention for their strong UV-light responsiveness, exceptional thermal stability, and theoretically predicted ultrahigh carrier mobility. In this study, we synthesized Pb and Sn-based <i>n</i> = 1 2D RP perovskite films covering millimeter-scale areas for the first time, utilizing a one-step chemical vapor deposition (CVD) method under atmospheric conditions. These films feature perovskite layers oriented horizontally relative to the substrate. Multilayered Cs<sub>3</sub>Pb<sub>2</sub>I<sub>3</sub>Cl<sub>4</sub> (Pb-based, <i>n</i> = 2) and Cs<sub>3</sub>Sn<sub>2</sub>I<sub>3</sub>Cl<sub>4</sub> (Sn-based, <i>n</i> = 2) films were also obtained for the first time, and their crystallographic structures were refined by combining X-ray diffraction (XRD) and density functional theory (DFT) calculations. DFT calculations and experimental optical spectroscopy support band-gap energy shifts related to the perovskite layer thickness. We demonstrate bias-free photodetectors using the Sn-based, <i>n</i> = 1 perovskite with reproducible photocurrent and a fast 84 ms response time. The present work not only demonstrates the growth of high-quality all-inorganic multilayered 2D perovskites via the CVD method but also suggests their potential as promising candidates for future optoelectronic applications.

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Publication Details

Journal
ACS Applied Materials & Interfaces
Published
2024-08-23
DOI
https://doi.org/10.1021/acsami.4c05329
Citations
6
Primary Topic
Perovskite Materials and Applications
Type
article
Field-Weighted Citation Impact
1.25

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article

Vapor Growth of All-Inorganic 2D Ruddlesden–Popper Lead- and Tin-Based Perovskites

Michael C. De Siena, Claudine Katan, Xinting Shuai, Anamika Mishra et al.
6 citations
ACS Applied Materials & Interfaces
Perovskite Materials and Applications
1.25
article

Vapor Growth of All-Inorganic 2D Ruddlesden–Popper Lead- and Tin-Based Perovskites

Michael C. De Siena, Claudine Katan, Xinting Shuai, Anamika Mishra, Laurent Pédesseau, Pulickel Madhavapanicker Ajayan, Aditya D. Mohite, Mercouri G. Kanatzidis, Róbert Vajtai, Anand B. Puthirath, Jacky Even, Ayush Agrawal, Yafei Wang, Xiang Zhang, Siraj Sidhik, Jianan Xu, Jin Hou, Jessica Persaud, Hao Zhang, Wenbin Li, Guanhui Gao, Mingrui Xu, Jeremy Daum
article en
6 citations

Abstract

The 2D Ruddlesden-Popper (RP) perovskites Cs<sub>2</sub>PbI<sub>2</sub>Cl<sub>2</sub> (Pb-based, <i>n</i> = 1) and Cs<sub>2</sub>SnI<sub>2</sub>Cl<sub>2</sub> (Sn-based, <i>n</i> = 1) stand out as unique and rare instances of entirely inorganic constituents within the more expansive category of organic/inorganic 2D perovskites. These materials have recently garnered significant attention for their strong UV-light responsiveness, exceptional thermal stability, and theoretically predicted ultrahigh carrier mobility. In this study, we synthesized Pb and Sn-based <i>n</i> = 1 2D RP perovskite films covering millimeter-scale areas for the first time, utilizing a one-step chemical vapor deposition (CVD) method under atmospheric conditions. These films feature perovskite layers oriented horizontally relative to the substrate. Multilayered Cs<sub>3</sub>Pb<sub>2</sub>I<sub>3</sub>Cl<sub>4</sub> (Pb-based, <i>n</i> = 2) and Cs<sub>3</sub>Sn<sub>2</sub>I<sub>3</sub>Cl<sub>4</sub> (Sn-based, <i>n</i> = 2) films were also obtained for the first time, and their crystallographic structures were refined by combining X-ray diffraction (XRD) and density functional theory (DFT) calculations. DFT calculations and experimental optical spectroscopy support band-gap energy shifts related to the perovskite layer thickness. We demonstrate bias-free photodetectors using the Sn-based, <i>n</i> = 1 perovskite with reproducible photocurrent and a fast 84 ms response time. The present work not only demonstrates the growth of high-quality all-inorganic multilayered 2D perovskites via the CVD method but also suggests their potential as promising candidates for future optoelectronic applications.

ACS Applied Materials & InterfacesVol. 16(35)
Northwestern University (US), Centre National de la Recherche Scientifique (FR), Institut National des Sciences Appliquées de Rennes (FR), Guangzhou University (CN), École Nationale Supérieure de Chimie de Rennes (FR), Fonctions Optiques pour les Technologies de l’information (FR), Université de Rennes (FR), Rice University (US)
U.S. Department of Energy, Northwestern University, European Commission, China Scholarship Council, Institut Universitaire de France, Grand Équipement National De Calcul Intensif, Office of Energy Efficiency and Renewable Energy, Office of Naval Research, Hydrogen and Fuel Cell Technologies Office, Office of Energy Efficiency, Institute of Circulatory and Respiratory Health, Office of Naval Research Global
Openalex Percentile: Top 20%
Perovskite Materials and Applications
1.25
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