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:

Fang, Yang ^[1]; Sojdak, Christopher A. ^[1]; Dey, Gangotri ^[1]; Teat, Simon J.  ^[2];

• Search DOE PAGES for author "Teat, Simon J."
• Search DOE PAGES for ORCID "0000-0001-9515-2602"

Li, Mingxing ^[3]; Cotlet, Mircea  ^[3];

• Search DOE PAGES for author "Cotlet, Mircea"
• Search DOE PAGES for ORCID "0000-0002-5024-3540"

Zhu, Kun ^[1]; Liu, Wei ^[4]; Wang, Lu  ^[1];

• Search DOE PAGES for author "Wang, Lu"
• Search DOE PAGES for ORCID "0000-0001-6230-1835"

ÓCarroll, Deirdre M.  ^[5];

• Search DOE PAGES for author "ÓCarroll, Deirdre M."
• Search DOE PAGES for ORCID "0000-0001-7209-4278"

Li, Jing  ^[6]

• Search DOE PAGES for author "Li, Jing"
• Search DOE PAGES for ORCID "0000-0001-7792-4322"

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+ Show Author Affiliations

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
6. Department of Chemistry and Chemical Biology; Rutgers University; Piscataway; USA

Publication Date:

Wed Apr 17 00:00:00 EDT 2019

Research Org.:

Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States); Rutgers Univ., Piscataway, NJ (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES); 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; CSHCBM; ark:/13030/qt42w9p2mq

Grant/Contract Number:  

AC02-05CH11231; SC0012704; DMR-1507210; TG-CHE170034

Resource Type:

Accepted Manuscript

Journal Name:

Chemical Science

Additional Journal Information:

Journal Volume: 10; Journal Issue: 20; 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