K2CuX3 (X = Cl, Br): All-Inorganic Lead-Free Blue Emitters with Near-Unity Photoluminescence Quantum Yield
Abstract
Recently, copper(I) halides have been gaining increased attention as highly luminescent nontoxic alternatives to lead halide perovskites for optoelectronic applications. In this paper, we report preparation of blue emitting, lead free, all-inorganic halides K2CuX3 (X = Cl, Br) through five synthetic methods including traditional solid-state and solution methods. The photoluminescence (PL) emission spectra of K2CuCl3 and K2CuBr3 exhibit narrow peaks centered at 392 and 388 nm with full widths at half-maximum (fwhm) values of ~54 nm. The visible bright blue emission is corroborated by the remarkably high photoluminescence quantum yield (PLQY) values up to ~97%. Furthermore, radioluminescence measurements on K2CuCl3 yield a bright peak at 404 nm under irradiation with X-rays at 200 kVp and 20 mA, which is optimal for use with PMTs and Si photomultipliers, suggesting a strong potential of this family for radiation detection applications. Based on our combined experimental and computational investigations, the origin of the efficient luminescence in K2CuX3 is attributed to the high stability self-trapped excitons (STE) formed in the one-dimensional anionic ∞1[CuX3]2– chains. Advantageously, K2CuX3 demonstrate improved air- and photostability compared to the previously reported copper(I) halides. The discovery of highly efficient and high stability light emitters based on earth-abundant copper(I) halides pavesmore »
- Authors:
-
- Univ. of Oklahoma, Norman, OK (United States). Dept. of Chemistry and Biochemistry
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Isotope and Fuel Cycle Technology Division
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
- 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). Materials Sciences & Engineering Division; Oklahoma Centerbfor the Advancement of Science and Technology; National Aeronautics and Space Administration (NASA); National Science Foundation (NSF)
- OSTI Identifier:
- 1649144
- Grant/Contract Number:
- AC05-00OR22725; AR18-008; 80NSSC19M0140; CHE-1726630
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 32; Journal Issue: 14; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; inorganic compounds; crystal structure; physical and chemical processes; photoluminescence; halogens; halide perovskites; copper(I) halides
Citation Formats
Creason, Tielyr D., McWhorter, Timothy M., Bell, Zane, Du, Mao-Hua, and Saparov, Bayrammurad. K2CuX3 (X = Cl, Br): All-Inorganic Lead-Free Blue Emitters with Near-Unity Photoluminescence Quantum Yield. United States: N. p., 2020.
Web. doi:10.1021/acs.chemmater.0c02098.
Creason, Tielyr D., McWhorter, Timothy M., Bell, Zane, Du, Mao-Hua, & Saparov, Bayrammurad. K2CuX3 (X = Cl, Br): All-Inorganic Lead-Free Blue Emitters with Near-Unity Photoluminescence Quantum Yield. United States. https://doi.org/10.1021/acs.chemmater.0c02098
Creason, Tielyr D., McWhorter, Timothy M., Bell, Zane, Du, Mao-Hua, and Saparov, Bayrammurad. 2020.
"K2CuX3 (X = Cl, Br): All-Inorganic Lead-Free Blue Emitters with Near-Unity Photoluminescence Quantum Yield". United States. https://doi.org/10.1021/acs.chemmater.0c02098. https://www.osti.gov/servlets/purl/1649144.
@article{osti_1649144,
title = {K2CuX3 (X = Cl, Br): All-Inorganic Lead-Free Blue Emitters with Near-Unity Photoluminescence Quantum Yield},
author = {Creason, Tielyr D. and McWhorter, Timothy M. and Bell, Zane and Du, Mao-Hua and Saparov, Bayrammurad},
abstractNote = {Recently, copper(I) halides have been gaining increased attention as highly luminescent nontoxic alternatives to lead halide perovskites for optoelectronic applications. In this paper, we report preparation of blue emitting, lead free, all-inorganic halides K2CuX3 (X = Cl, Br) through five synthetic methods including traditional solid-state and solution methods. The photoluminescence (PL) emission spectra of K2CuCl3 and K2CuBr3 exhibit narrow peaks centered at 392 and 388 nm with full widths at half-maximum (fwhm) values of ~54 nm. The visible bright blue emission is corroborated by the remarkably high photoluminescence quantum yield (PLQY) values up to ~97%. Furthermore, radioluminescence measurements on K2CuCl3 yield a bright peak at 404 nm under irradiation with X-rays at 200 kVp and 20 mA, which is optimal for use with PMTs and Si photomultipliers, suggesting a strong potential of this family for radiation detection applications. Based on our combined experimental and computational investigations, the origin of the efficient luminescence in K2CuX3 is attributed to the high stability self-trapped excitons (STE) formed in the one-dimensional anionic ∞1[CuX3]2– chains. Advantageously, K2CuX3 demonstrate improved air- and photostability compared to the previously reported copper(I) halides. The discovery of highly efficient and high stability light emitters based on earth-abundant copper(I) halides paves the way for their potential practical applications.},
doi = {10.1021/acs.chemmater.0c02098},
url = {https://www.osti.gov/biblio/1649144},
journal = {Chemistry of Materials},
issn = {0897-4756},
number = 14,
volume = 32,
place = {United States},
year = {Mon Jun 22 00:00:00 EDT 2020},
month = {Mon Jun 22 00:00:00 EDT 2020}
}
Web of Science
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