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Title: High Layer Number (n = 1–6) 2D Ruddlesden–Popper Lead Bromide Perovskites: Nanosheets, Crystal Structure, and Optoelectronic Properties

Abstract

2D Ruddlesden–Popper (RP) lead halide perovskites have highly tunable structures, compositions, and properties that enable their promising optoelectronic applications. Among various 2D halide perovskites, the materials chemistry and fundamental optoelectronic properties of high layer number (n) lead-bromide RP perovskites, where n refers to the number of inorganic octahedra layers, have been less studied. Here, we report the synthesis of thin nanosheets of (PEA)2Csn–1PbnBr3n+1 (n = 1–6, PEA = phenylethylammonium) perovskites and study the optical properties, assigning photoluminescence emissions of 486, 496, and 505 nm to n = 4–6 phases, respectively, and reporting the photoluminescence lifetimes. Furthermore, the crystal structure of (PEA)2Cs2Pb3Br10 was determined to reveal minimal octahedral structural distortions. Ultraviolet photoelectron spectroscopy measurements reveal the positioning of the valence and conduction bands for n = 1–3 phases and confirm the type-I band alignment for the (PEA)2Csn–1PbnBr3n+1 series, laying the foundation for rational heterostructure device design in the future.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]
  1. University of Wisconsin─Madison, WI (United States)
  2. University of Kentucky, Lexington, KY (United States)
Publication Date:
Research Org.:
Univ. of Kentucky, Lexington, KY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
2205086
Grant/Contract Number:  
SC0018208; SC0002162
Resource Type:
Accepted Manuscript
Journal Name:
ACS Materials Letters
Additional Journal Information:
Journal Volume: 5; Journal Issue: 11; Journal ID: ISSN 2639-4979
Publisher:
ACS Publications
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Absorption; Anions; Crystal structure; Perovskites; Two dimensional materials

Citation Formats

Forlano, Kristel M., Roy, Chris R., Mihalyi-Koch, Willa, Hossain, Tareq, Sanders, Kyana, Guzei, Ilia, Graham, Kenneth R., Wright, John C., and Jin, Song. High Layer Number (n = 1–6) 2D Ruddlesden–Popper Lead Bromide Perovskites: Nanosheets, Crystal Structure, and Optoelectronic Properties. United States: N. p., 2023. Web. doi:10.1021/acsmaterialslett.3c00809.
Forlano, Kristel M., Roy, Chris R., Mihalyi-Koch, Willa, Hossain, Tareq, Sanders, Kyana, Guzei, Ilia, Graham, Kenneth R., Wright, John C., & Jin, Song. High Layer Number (n = 1–6) 2D Ruddlesden–Popper Lead Bromide Perovskites: Nanosheets, Crystal Structure, and Optoelectronic Properties. United States. https://doi.org/10.1021/acsmaterialslett.3c00809
Forlano, Kristel M., Roy, Chris R., Mihalyi-Koch, Willa, Hossain, Tareq, Sanders, Kyana, Guzei, Ilia, Graham, Kenneth R., Wright, John C., and Jin, Song. Thu . "High Layer Number (n = 1–6) 2D Ruddlesden–Popper Lead Bromide Perovskites: Nanosheets, Crystal Structure, and Optoelectronic Properties". United States. https://doi.org/10.1021/acsmaterialslett.3c00809.
@article{osti_2205086,
title = {High Layer Number (n = 1–6) 2D Ruddlesden–Popper Lead Bromide Perovskites: Nanosheets, Crystal Structure, and Optoelectronic Properties},
author = {Forlano, Kristel M. and Roy, Chris R. and Mihalyi-Koch, Willa and Hossain, Tareq and Sanders, Kyana and Guzei, Ilia and Graham, Kenneth R. and Wright, John C. and Jin, Song},
abstractNote = {2D Ruddlesden–Popper (RP) lead halide perovskites have highly tunable structures, compositions, and properties that enable their promising optoelectronic applications. Among various 2D halide perovskites, the materials chemistry and fundamental optoelectronic properties of high layer number (n) lead-bromide RP perovskites, where n refers to the number of inorganic octahedra layers, have been less studied. Here, we report the synthesis of thin nanosheets of (PEA)2Csn–1PbnBr3n+1 (n = 1–6, PEA = phenylethylammonium) perovskites and study the optical properties, assigning photoluminescence emissions of 486, 496, and 505 nm to n = 4–6 phases, respectively, and reporting the photoluminescence lifetimes. Furthermore, the crystal structure of (PEA)2Cs2Pb3Br10 was determined to reveal minimal octahedral structural distortions. Ultraviolet photoelectron spectroscopy measurements reveal the positioning of the valence and conduction bands for n = 1–3 phases and confirm the type-I band alignment for the (PEA)2Csn–1PbnBr3n+1 series, laying the foundation for rational heterostructure device design in the future.},
doi = {10.1021/acsmaterialslett.3c00809},
journal = {ACS Materials Letters},
number = 11,
volume = 5,
place = {United States},
year = {Thu Sep 28 00:00:00 EDT 2023},
month = {Thu Sep 28 00:00:00 EDT 2023}
}

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