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Stimuli-responsive Photoluminescent Copper(I) Halides for Scintillation, Anticounterfeiting and LED Applications
  • +6
  • Bayram Saparov,
  • Dilruba A. Popy,
  • Yashpal Singh,
  • Yauhen Tratsiak,
  • Abby M. Cardoza,
  • John M. Lane,
  • Luis Stand,
  • Mariya Zhuravleva,
  • Neeraj Rai
Bayram Saparov
The University of Oklahoma Department of Chemistry and Biochemistry

Corresponding Author:saparov@ou.edu

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Dilruba A. Popy
The University of Oklahoma Department of Chemistry and Biochemistry
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Yashpal Singh
Mississippi State University Dave C Swalm School of Chemical Engineering
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Yauhen Tratsiak
The University of Tennessee Knoxville
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Abby M. Cardoza
The University of Oklahoma Department of Chemistry and Biochemistry
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John M. Lane
Mississippi State University Dave C Swalm School of Chemical Engineering
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Luis Stand
The University of Tennessee Knoxville
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Mariya Zhuravleva
The University of Tennessee Knoxville
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Neeraj Rai
Mississippi State University Dave C Swalm School of Chemical Engineering
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Abstract

Highly sensitive stimuli-responsive multifunctional luminescent materials are crucial for applications in optical sensing, high-level security, and anticounterfeiting. Here, we report two zero-dimensional (0D) hybrid copper(I) halides, (TEP) 2Cu 2Br 4 and (TEP) 2Cu 4Br 6, which are comprised of isolated [Cu 2Br 4] 2- and [Cu 4Br 6] 2- inorganic cluster units, respectively, separated by TEP + (TEP = tetraethylphosphonium) cations. (TEP) 2Cu 2Br 4 and (TEP) 2Cu 4Br 6 demonstrate ultrabright greenish-white and orange-red emissions, respectively, with near unity photoluminescence quantum yields. Optical spectroscopy measurements and density-functional theory (DFT) calculations reveal that photoemissions of these compounds originate from the formation of self-trapped excitons (STEs) due to the excited-state distortions in the copper(I) halide units. Single crystals of both compounds are radioluminescence (RL) active at room temperature under both X- and γ-rays exposure. The excellent energy resolution values and light yields up to 15,800 ph/MeV under 662 keV γ-rays of 137Cs suggest their potential for scintillation applications. Remarkably, (TEP) 2Cu 2Br 4 and (TEP) 2Cu 4Br 6 are interconvertible through external chemical stimuli or reverse crystallization. In addition, both compounds demonstrate luminescence on-off switching upon thermal stimuli. The sensitivity of (TEP) 2Cu 2Br 4 and (TEP) 2Cu 4Br 6 to the chemical and thermal stimuli coupled with their ultrabright emission allows their consideration for practical applications such as solid-state lighting, sensing, information storage, and anticounterfeiting.
31 Jan 2024Submitted to Aggregate
31 Jan 2024Submission Checks Completed
31 Jan 2024Assigned to Editor
17 Feb 2024Review(s) Completed, Editorial Evaluation Pending
18 Mar 20241st Revision Received
18 Mar 2024Submission Checks Completed
18 Mar 2024Assigned to Editor
28 Mar 2024Review(s) Completed, Editorial Evaluation Pending
31 Mar 2024Editorial Decision: Revise Major
16 Apr 20242nd Revision Received
17 Apr 2024Reviewer(s) Assigned
11 May 2024Review(s) Completed, Editorial Evaluation Pending
16 May 2024Review(s) Completed, Editorial Evaluation Pending
16 May 2024Editorial Decision: Accept