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Title: Highly efficient and very robust blue-excitable yellow phosphors built on multiple-stranded one-dimensional inorganic–organic hybrid chains

Abstract

Inorganic–organic hybrid semiconductors are promising candidates for energy-related applications. Here, we have developed a unique class of multiple-stranded one-dimensional (1D) structures as very robust and efficient lighting phosphors. Following a systematic ligand design strategy, these structures are constructed by forming multiple coordination bonds between adjacent copper iodide inorganic building units Cu mI m (m = 2, 4, 6) (e.g. dimer, tetramer and hexamer clusters) and strong-binding bidentate organic ligands with low LUMO energies which give rise to infinite 1D chains of high stability and low bandgaps. The significantly enhanced thermal/photostability of these multiple-stranded chain structures is largely attributed to the multi-dentate nature and enhanced Cu–N bonding, and their excellent blue excitability is a result of using benzotriazole based ligands with low-lying LUMO energies. These facts are confirmed by Density Functional Theory (DFT) calculations. The luminescence mechanism of these compounds is studied by temperature dependent photoluminescence experiments. High internal quantum yields (IQYs) are achieved under blue excitation, marking the highest value reported so far for crystalline inorganic–organic hybrid yellow phosphors. Excellent thermal- and photo-stability, coupled with high luminescence efficiency, make this class of materials promising candidates for use as rare-earth element (REE) free phosphors in energy efficient general lighting devices.

Authors:
 [1];  [1];  [1]; ORCiD logo [2];  [3]; ORCiD logo [3];  [1];  [4]; ORCiD logo [1]; ORCiD logo [5]; ORCiD logo [1]
  1. Rutgers Univ., Piscataway, NJ (United States). Dept. of Chemistry and Chemical Biology
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
  4. Shenzhen Polytechnic (China). Hoffman Inst. of Advanced Materials
  5. Rutgers Univ., Piscataway, NJ (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Rutgers Univ., Piscataway, NJ (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1572815
Alternate Identifier(s):
OSTI ID: 1513220
Report Number(s):
BNL-211596-2019-JAAM
Journal ID: ISSN 2041-6520
Grant/Contract Number:  
SC0012704; AC02-05CH11231; DMR-1507210; TG-CHE170034
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Science
Additional Journal Information:
Journal Name: Chemical Science; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Fang, Yang, Sojdak, Christopher A., Dey, Gangotri, Teat, Simon J., Li, Mingxing, Cotlet, Mircea, Zhu, Kun, Liu, Wei, Wang, Lu, ÓCarroll, Deirdre M., and Li, Jing. Highly efficient and very robust blue-excitable yellow phosphors built on multiple-stranded one-dimensional inorganic–organic hybrid chains. United States: N. p., 2019. Web. doi:10.1039/C9SC00970A.
Fang, Yang, Sojdak, Christopher A., Dey, Gangotri, Teat, Simon J., Li, Mingxing, Cotlet, Mircea, Zhu, Kun, Liu, Wei, Wang, Lu, ÓCarroll, Deirdre M., & Li, Jing. Highly efficient and very robust blue-excitable yellow phosphors built on multiple-stranded one-dimensional inorganic–organic hybrid chains. United States. doi:10.1039/C9SC00970A.
Fang, Yang, Sojdak, Christopher A., Dey, Gangotri, Teat, Simon J., Li, Mingxing, Cotlet, Mircea, Zhu, Kun, Liu, Wei, Wang, Lu, ÓCarroll, Deirdre M., and Li, Jing. Wed . "Highly efficient and very robust blue-excitable yellow phosphors built on multiple-stranded one-dimensional inorganic–organic hybrid chains". United States. doi:10.1039/C9SC00970A. https://www.osti.gov/servlets/purl/1572815.
@article{osti_1572815,
title = {Highly efficient and very robust blue-excitable yellow phosphors built on multiple-stranded one-dimensional inorganic–organic hybrid chains},
author = {Fang, Yang and Sojdak, Christopher A. and Dey, Gangotri and Teat, Simon J. and Li, Mingxing and Cotlet, Mircea and Zhu, Kun and Liu, Wei and Wang, Lu and ÓCarroll, Deirdre M. and Li, Jing},
abstractNote = {Inorganic–organic hybrid semiconductors are promising candidates for energy-related applications. Here, we have developed a unique class of multiple-stranded one-dimensional (1D) structures as very robust and efficient lighting phosphors. Following a systematic ligand design strategy, these structures are constructed by forming multiple coordination bonds between adjacent copper iodide inorganic building units CumIm (m = 2, 4, 6) (e.g. dimer, tetramer and hexamer clusters) and strong-binding bidentate organic ligands with low LUMO energies which give rise to infinite 1D chains of high stability and low bandgaps. The significantly enhanced thermal/photostability of these multiple-stranded chain structures is largely attributed to the multi-dentate nature and enhanced Cu–N bonding, and their excellent blue excitability is a result of using benzotriazole based ligands with low-lying LUMO energies. These facts are confirmed by Density Functional Theory (DFT) calculations. The luminescence mechanism of these compounds is studied by temperature dependent photoluminescence experiments. High internal quantum yields (IQYs) are achieved under blue excitation, marking the highest value reported so far for crystalline inorganic–organic hybrid yellow phosphors. Excellent thermal- and photo-stability, coupled with high luminescence efficiency, make this class of materials promising candidates for use as rare-earth element (REE) free phosphors in energy efficient general lighting devices.},
doi = {10.1039/C9SC00970A},
journal = {Chemical Science},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {4}
}

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Figures / Tables:

Fig. 1 Fig. 1: Schematic illustrating the design and construction of 1D multiple-stranded hybrid structures: a) 1D single-stranded structure based on Cu2I2 dimer. b) 1D single-stranded structure based on Cu4I4 tetramer. c) 1D single-stranded structure based on Cu6I6 hexamer. d) 1D double-stranded structure based on Cu2I2 dimer. e) 1D double-stranded structure basedmore » on Cu4I4 tetramer. f) 1D triple-stranded structure based on Cu6I6 hexamer. Color scheme of the balls: cyan: Cu, pink: I, orange and blue rod (organic ligand).« less

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    • DOI: 10.1016/j.ccr.2016.06.016

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    • Leitl, Markus J.; Krylova, Valentina A.; Djurovich, Peter I.
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    • DOI: 10.1021/ja508155x

    One-dimensional organic lead halide perovskites with efficient bluish white-light emission
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    • DOI: 10.1038/ncomms14051

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    • DOI: 10.1021/cg101321u

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      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.