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Title: 0D and 2D: The Cases of Phenylethylammonium Tin Bromide Hybrids

Abstract

Tin halide perovskites and perovskite-related materials have emerged as promising lead-free hybrid materials for various optoelectronic applications. While remarkable progress has been achieved in the development of organic tin halide hybrids with diverse structures and controlled dimensionalities at the molecular level, some controversial results that have been reported recently need to be addressed. For instance, different photophysical properties have been reported for two-dimensional (2D) (PEA) 2SnBr 4 (PEA = phenylethylammonium) by several groups with distinct emission peaks at around 468 and 550 nm. Here we report our efforts in the synthesis of phenylethylammonium tin bromide hybrids with zero-dimensional (0D) and 2D structures, and characterizations of their structural and photophysical properties. 0D [(PEA) 4SnBr 6][(PEA)Br] 2[CCl 2H 2] 2 was found to exhibit strong yellow emission peak at 566 nm with a photoluminescence quantum efficiency (PLQE) of ~90%, while 2D (PEA) 2SnBr 4 had weak emission peak at 470 nm with a PLQE of <0.1%. Interestingly, 0D [(PEA) 4SnBr 6][(PEA)Br] 2[CCl 2H 2] 2 can be converted into 2D (PEA) 2SnBr 4 upon drying, which would return to 0D [(PEA) 4SnBr 6][(PEA)Br] 2[CCl 2H 2] 2 upon addition of dichloromethane. Powder X-ray diffraction results confirmed the reversible transformation between 0D andmore » 2D structures. Density functional theory calculations showed that excitons in 0D [(PEA) 4SnBr 6][(PEA)Br] 2[CCl 2H 2] 2 are highly localized, resulting in a strongly Stokes shifted broadband emission, while delocalized electronic states in 2D (PEA) 2SnBr 4 result in weaker exciton binding, a higher exciton mobility, and a higher nonradiative decay.« less

Authors:
 [1];  [1];  [1]; ORCiD logo [1];  [1];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Florida State Univ., Tallahassee, FL (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1649412
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 32; Journal Issue: 11; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Xu, Liang-Jin, Lin, Haoran, Lee, Sujin, Zhou, Chenkun, Worku, Michael, Chaaban, Maya, He, Qingquan, Plaviak, Anna, Lin, Xinsong, Chen, Banghao, Du, Mao-Hua, and Ma, Biwu. 0D and 2D: The Cases of Phenylethylammonium Tin Bromide Hybrids. United States: N. p., 2020. Web. doi:10.1021/acs.chemmater.0c01254.
Xu, Liang-Jin, Lin, Haoran, Lee, Sujin, Zhou, Chenkun, Worku, Michael, Chaaban, Maya, He, Qingquan, Plaviak, Anna, Lin, Xinsong, Chen, Banghao, Du, Mao-Hua, & Ma, Biwu. 0D and 2D: The Cases of Phenylethylammonium Tin Bromide Hybrids. United States. doi:10.1021/acs.chemmater.0c01254.
Xu, Liang-Jin, Lin, Haoran, Lee, Sujin, Zhou, Chenkun, Worku, Michael, Chaaban, Maya, He, Qingquan, Plaviak, Anna, Lin, Xinsong, Chen, Banghao, Du, Mao-Hua, and Ma, Biwu. Tue . "0D and 2D: The Cases of Phenylethylammonium Tin Bromide Hybrids". United States. doi:10.1021/acs.chemmater.0c01254.
@article{osti_1649412,
title = {0D and 2D: The Cases of Phenylethylammonium Tin Bromide Hybrids},
author = {Xu, Liang-Jin and Lin, Haoran and Lee, Sujin and Zhou, Chenkun and Worku, Michael and Chaaban, Maya and He, Qingquan and Plaviak, Anna and Lin, Xinsong and Chen, Banghao and Du, Mao-Hua and Ma, Biwu},
abstractNote = {Tin halide perovskites and perovskite-related materials have emerged as promising lead-free hybrid materials for various optoelectronic applications. While remarkable progress has been achieved in the development of organic tin halide hybrids with diverse structures and controlled dimensionalities at the molecular level, some controversial results that have been reported recently need to be addressed. For instance, different photophysical properties have been reported for two-dimensional (2D) (PEA)2SnBr4 (PEA = phenylethylammonium) by several groups with distinct emission peaks at around 468 and 550 nm. Here we report our efforts in the synthesis of phenylethylammonium tin bromide hybrids with zero-dimensional (0D) and 2D structures, and characterizations of their structural and photophysical properties. 0D [(PEA)4SnBr6][(PEA)Br]2[CCl2H2]2 was found to exhibit strong yellow emission peak at 566 nm with a photoluminescence quantum efficiency (PLQE) of ~90%, while 2D (PEA)2SnBr4 had weak emission peak at 470 nm with a PLQE of <0.1%. Interestingly, 0D [(PEA)4SnBr6][(PEA)Br]2[CCl2H2]2 can be converted into 2D (PEA)2SnBr4 upon drying, which would return to 0D [(PEA)4SnBr6][(PEA)Br]2[CCl2H2]2 upon addition of dichloromethane. Powder X-ray diffraction results confirmed the reversible transformation between 0D and 2D structures. Density functional theory calculations showed that excitons in 0D [(PEA)4SnBr6][(PEA)Br]2[CCl2H2]2 are highly localized, resulting in a strongly Stokes shifted broadband emission, while delocalized electronic states in 2D (PEA)2SnBr4 result in weaker exciton binding, a higher exciton mobility, and a higher nonradiative decay.},
doi = {10.1021/acs.chemmater.0c01254},
journal = {Chemistry of Materials},
issn = {0897-4756},
number = 11,
volume = 32,
place = {United States},
year = {2020},
month = {5}
}

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