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

Xinting Shuai; Siraj Sidhik; Mingrui Xu; Xiang Zhang; Michael De Siena; Laurent Pedesseau; Hao Zhang; Guanhui Gao; Anand B. Puthirath; Wenbin Li; Ayush Agrawal; Jianan Xu; Jin Hou; Jessica H. Persaud; Jeremy Daum; Anamika Mishra; Yafei Wang; Robert Vajtai; Claudine Katan; Mercouri G. Kanatzidis; Jacky Even; Pulickel M. Ajayan; Aditya D. Mohite

doi:10.1021/acsami.4c05329

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

Xinting Shuai, Siraj Sidhik, Mingrui Xu, Xiang Zhang, Michael De Siena, Laurent Pedesseau, Hao Zhang, Guanhui Gao, Anand B. Puthirath, Wenbin Li, Ayush Agrawal, Jianan Xu, Jin Hou, Jessica H. Persaud, Jeremy Daum, Anamika Mishra, Yafei Wang, Robert Vajtai, Claudine Katan, Mercouri G. KanatzidisJacky Even, Pulickel M. Ajayan^*, Aditya D. Mohite^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

1 Scopus citations

Abstract

The 2D Ruddlesden-Popper (RP) perovskites Cs₂PbI₂Cl₂ (Pb-based, n = 1) and Cs₂SnI₂Cl₂ (Sn-based, n = 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 n = 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 Cs₃Pb₂I₃Cl₄ (Pb-based, n = 2) and Cs₃Sn₂I₃Cl₄ (Sn-based, n = 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, n = 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.

Original language	English (US)
Pages (from-to)	46560-46569
Number of pages	10
Journal	ACS Applied Materials and Interfaces
Volume	16
Issue number	35
DOIs	https://doi.org/10.1021/acsami.4c05329
State	Published - Sep 4 2024

Funding

A.D.M. and X.S. acknowledge research support from the HydroGEN Advanced Water Splitting Materials Consortium, established as part of the Energy Materials Network under the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Hydrogen and Fuel Cell Technologies Office, under the Award No. DE-EE0008843. J.H. acknowledges the financial support from the China Scholarships Council (No. 202107990007). The work at ISCR and FOTON was supported by the European Union\u2019s Horizon 2020 Research and Innovation Program, under Grant Agreement No. 861985 (PeroCUBE). J.E. acknowledges the financial support from the Institut Universitaire de France. This work was granted access to the HPC resources of TGCC/CINES under Allocation No. A0140911434 made by GENCI. At Northwestern, this work was supported by the Office of Naval Research (ONR), under Grant No. N00014-20-1-2725. The authors acknowledge the support from Esther Tsai for her assistance in performing GIWAXS measurements at the BNL beamline.

Keywords

2D perovskites
CVD
all-inorganic perovskites
photodetector
tin-based perovskites

ASJC Scopus subject areas

General Materials Science

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10.1021/acsami.4c05329

Cite this

Shuai, X., Sidhik, S., Xu, M., Zhang, X., De Siena, M., Pedesseau, L., Zhang, H., Gao, G., Puthirath, A. B., Li, W., Agrawal, A., Xu, J., Hou, J., Persaud, J. H., Daum, J., Mishra, A., Wang, Y., Vajtai, R., Katan, C., ... Mohite, A. D. (2024). Vapor Growth of All-Inorganic 2D Ruddlesden-Popper Lead- and Tin-Based Perovskites. ACS Applied Materials and Interfaces, 16(35), 46560-46569. https://doi.org/10.1021/acsami.4c05329

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title = "Vapor Growth of All-Inorganic 2D Ruddlesden-Popper Lead- and Tin-Based Perovskites",

abstract = "The 2D Ruddlesden-Popper (RP) perovskites Cs2PbI2Cl2 (Pb-based, n = 1) and Cs2SnI2Cl2 (Sn-based, n = 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 n = 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 Cs3Pb2I3Cl4 (Pb-based, n = 2) and Cs3Sn2I3Cl4 (Sn-based, n = 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, n = 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.",

keywords = "2D perovskites, CVD, all-inorganic perovskites, photodetector, tin-based perovskites",

author = "Xinting Shuai and Siraj Sidhik and Mingrui Xu and Xiang Zhang and {De Siena}, Michael and Laurent Pedesseau and Hao Zhang and Guanhui Gao and Puthirath, {Anand B.} and Wenbin Li and Ayush Agrawal and Jianan Xu and Jin Hou and Persaud, {Jessica H.} and Jeremy Daum and Anamika Mishra and Yafei Wang and Robert Vajtai and Claudine Katan and Kanatzidis, {Mercouri G.} and Jacky Even and Ajayan, {Pulickel M.} and Mohite, {Aditya D.}",

note = "Publisher Copyright: {\textcopyright} 2024 American Chemical Society.",

year = "2024",

month = sep,

day = "4",

doi = "10.1021/acsami.4c05329",

language = "English (US)",

volume = "16",

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journal = "ACS Applied Materials and Interfaces",

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Shuai, X, Sidhik, S, Xu, M, Zhang, X, De Siena, M, Pedesseau, L, Zhang, H, Gao, G, Puthirath, AB, Li, W, Agrawal, A, Xu, J, Hou, J, Persaud, JH, Daum, J, Mishra, A, Wang, Y, Vajtai, R, Katan, C, Kanatzidis, MG, Even, J, Ajayan, PM & Mohite, AD 2024, 'Vapor Growth of All-Inorganic 2D Ruddlesden-Popper Lead- and Tin-Based Perovskites', ACS Applied Materials and Interfaces, vol. 16, no. 35, pp. 46560-46569. https://doi.org/10.1021/acsami.4c05329

TY - JOUR

T1 - Vapor Growth of All-Inorganic 2D Ruddlesden-Popper Lead- and Tin-Based Perovskites

AU - Shuai, Xinting

AU - Sidhik, Siraj

AU - Xu, Mingrui

AU - Zhang, Xiang

AU - De Siena, Michael

AU - Pedesseau, Laurent

AU - Zhang, Hao

AU - Gao, Guanhui

AU - Puthirath, Anand B.

AU - Li, Wenbin

AU - Agrawal, Ayush

AU - Xu, Jianan

AU - Hou, Jin

AU - Persaud, Jessica H.

AU - Daum, Jeremy

AU - Mishra, Anamika

AU - Wang, Yafei

AU - Vajtai, Robert

AU - Katan, Claudine

AU - Kanatzidis, Mercouri G.

AU - Even, Jacky

AU - Ajayan, Pulickel M.

AU - Mohite, Aditya D.

PY - 2024/9/4

Y1 - 2024/9/4

N2 - The 2D Ruddlesden-Popper (RP) perovskites Cs2PbI2Cl2 (Pb-based, n = 1) and Cs2SnI2Cl2 (Sn-based, n = 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 n = 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 Cs3Pb2I3Cl4 (Pb-based, n = 2) and Cs3Sn2I3Cl4 (Sn-based, n = 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, n = 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.

AB - The 2D Ruddlesden-Popper (RP) perovskites Cs2PbI2Cl2 (Pb-based, n = 1) and Cs2SnI2Cl2 (Sn-based, n = 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 n = 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 Cs3Pb2I3Cl4 (Pb-based, n = 2) and Cs3Sn2I3Cl4 (Sn-based, n = 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, n = 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.

KW - 2D perovskites

KW - CVD

KW - all-inorganic perovskites

KW - photodetector

KW - tin-based perovskites

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DO - 10.1021/acsami.4c05329

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SN - 1944-8244

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EP - 46569

JO - ACS Applied Materials and Interfaces

JF - ACS Applied Materials and Interfaces

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ER -

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

Abstract

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