A One-Dimensional Organic Lead Chloride Hybrid with Excitation-Dependent Broadband Emissions

Guanhong Wu; Chenkun Zhou; Wenmei Ming; Dan Han; Shiyou Chen; Dong Yang; Tiglet Besara; Jennifer Neu; Theo Siegrist; Mao Hua Du; Biwu Ma; Angang Dong

doi:10.1021/acsenergylett.8b00661

A One-Dimensional Organic Lead Chloride Hybrid with Excitation-Dependent Broadband Emissions

Guanhong Wu, Chenkun Zhou, Wenmei Ming, Dan Han, Shiyou Chen, Dong Yang, Tiglet Besara, Jennifer Neu, Theo Siegrist, Mao Hua Du, Biwu Ma, Angang Dong

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

134 Scopus citations

Abstract

Organic-inorganic metal halide hybrids have emerged as a new class of materials with fascinating optical and electronic properties. The exceptional structure tunability has enabled the development of materials with various dimensionalities at the molecular level, from three-dimensional (3D) to 2D, 1D, and 0D. Here, we report a new 1D lead chloride hybrid, C₄N₂H₁₄PbCl₄, which exhibits unusual inverse excitation-dependent broadband emission from bluish-green to yellow. Density functional theory calculations were performed to better understand the mechanism of this excitation-dependent broadband emission. This 1D hybrid material is found to have two emission centers, corresponding to the self-trapped excitons (STEs) and vacancy-bound excitons. The excitation-dependent emission is due to different populations of these two types of excitons generated at different excitation wavelengths. This work shows the rich chemistry and physics of organic-inorganic metal halide hybrids and paves the way to achieving novel light emitters with excitation-dependent broadband emissions at room temperature.

Original language	English
Pages (from-to)	1443-1449
Number of pages	7
Journal	ACS Energy Letters
Volume	3
Issue number	6
DOIs	https://doi.org/10.1021/acsenergylett.8b00661
State	Published - Jun 8 2018
Externally published	Yes

Funding

A.D. acknowledges support from MOST (2017YFA0207303, 2014CB845602), Key Basic Research Program of Science and Technology Commission of Shanghai Municipality (17JC1400100), Shanghai International Science and Technology Cooperation Project (15520720100), and NSFC (21733003). C.Z. and B.M. acknowledge the support from the National Science Foundation (DMR-1709116 and CHE-1664661). B.M. also acknowledges support from the Senior Visiting Scholar Foundation of Key Laboratory at Fudan University. The work at ORNL was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences, and Engineering Division. D.H. and S.C. were supported by NSFC under Grant Nos. 61574059 and 61722402, Shu-Guang program (15SG20), and CC of ECNU. This manuscript has been co-authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/ downloads/doe-public-access-plan).

Funders	Funder number
National Science Foundation	1531629, 1709116
Ministry of Science and Technology of the People's Republic of China

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abstract = "Organic-inorganic metal halide hybrids have emerged as a new class of materials with fascinating optical and electronic properties. The exceptional structure tunability has enabled the development of materials with various dimensionalities at the molecular level, from three-dimensional (3D) to 2D, 1D, and 0D. Here, we report a new 1D lead chloride hybrid, C4N2H14PbCl4, which exhibits unusual inverse excitation-dependent broadband emission from bluish-green to yellow. Density functional theory calculations were performed to better understand the mechanism of this excitation-dependent broadband emission. This 1D hybrid material is found to have two emission centers, corresponding to the self-trapped excitons (STEs) and vacancy-bound excitons. The excitation-dependent emission is due to different populations of these two types of excitons generated at different excitation wavelengths. This work shows the rich chemistry and physics of organic-inorganic metal halide hybrids and paves the way to achieving novel light emitters with excitation-dependent broadband emissions at room temperature.",

author = "Guanhong Wu and Chenkun Zhou and Wenmei Ming and Dan Han and Shiyou Chen and Dong Yang and Tiglet Besara and Jennifer Neu and Theo Siegrist and Du, {Mao Hua} and Biwu Ma and Angang Dong",

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AU - Chen, Shiyou

AU - Yang, Dong

AU - Besara, Tiglet

AU - Neu, Jennifer

AU - Siegrist, Theo

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AU - Ma, Biwu

AU - Dong, Angang

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N2 - Organic-inorganic metal halide hybrids have emerged as a new class of materials with fascinating optical and electronic properties. The exceptional structure tunability has enabled the development of materials with various dimensionalities at the molecular level, from three-dimensional (3D) to 2D, 1D, and 0D. Here, we report a new 1D lead chloride hybrid, C4N2H14PbCl4, which exhibits unusual inverse excitation-dependent broadband emission from bluish-green to yellow. Density functional theory calculations were performed to better understand the mechanism of this excitation-dependent broadband emission. This 1D hybrid material is found to have two emission centers, corresponding to the self-trapped excitons (STEs) and vacancy-bound excitons. The excitation-dependent emission is due to different populations of these two types of excitons generated at different excitation wavelengths. This work shows the rich chemistry and physics of organic-inorganic metal halide hybrids and paves the way to achieving novel light emitters with excitation-dependent broadband emissions at room temperature.

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A One-Dimensional Organic Lead Chloride Hybrid with Excitation-Dependent Broadband Emissions

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