Luminescence from Self‐Trapped Excitons and Energy Transfers in Vacancy‐Ordered Hexagonal Halide Perovskite Cs 2 HfF 6 Doped with Rare Earths for Radiation Detection
Abstract
Compared to halides Cs2HfX6 (X = Cl, Br, I) with a vacancy-ordered cubic double perovskite structure, the halide Cs2HfF6 (CHF), with a hexagonal Bravais lattice, possesses a higher mass density and chemical stability for radiation detection. Luminescence properties and energy transfer mechanisms of rare-earths-doped CHF materials are studied here. The structure of CHF is identified as a new type of vacancy-ordered hexagonal perovskite, with the same type of building blocks of the double perovskite but stacked with single layers. Density-functional theory calculations reveal a large bandgap of CHF. A broad emission is observed from the pristine CHF host, which is suggested to be associated with self-trapped excitons (STEs). A series of rare-earths-doped materials are designed utilizing the STE emissions, and efficient energy transfers from STEs and Tb3+ to Eu3+ are achieved for tunable emissions. The codoped material shows stable emission under X-ray irradiation, with 10.2% reduction from its initial emission intensity, associated with possible structural evolution by radiation-induced deformation of the soft host. The radiation responses of singly and codoped materials are evaluated, and the codoped material is found to be more sensitive to the radiation energy than the singly doped or pristine CHF for radiation detection.
- Authors:
-
[1];
[1];
[2];
[1]
- Department of Chemistry, Physics and Materials Science Fayetteville State University Fayetteville NC 28301 USA
- X‐Ray Science Division Argonne National Laboratory Lemont IL 60439 USA
- Computational Sciences and Engineering Division Oak Ridge National Laboratory Oak Ridge TN 37831 USA
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Nuclear Energy (NE); National Science Foundation (NSF); USDOD
- OSTI Identifier:
- 1881541
- Alternate Identifier(s):
- OSTI ID: 1883843; OSTI ID: 1891180; OSTI ID: 1970717
- Grant/Contract Number:
- AC05-00OR22725; W911NF-09-1-0011; ECCS-1900837; DMR-1626376; AC02-06CH11357; AC02-05CH11231; AC07-05ID14517
- Resource Type:
- Published Article
- Journal Name:
- Advanced Optical Materials
- Additional Journal Information:
- Journal Name: Advanced Optical Materials Journal Volume: 10 Journal Issue: 19; Journal ID: ISSN 2195-1071
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; fluorides; halides; luminescence; perovskites; phosphors; radiation detection
Citation Formats
Adhikari, Menuka, Shrivastava, Navadeep, McClain, Starfari T., Adhikari, Chandra M., Guzelturk, Burak, Khanal, Rabi, Gautam, Bhoj, and Luo, Zhiping. Luminescence from Self‐Trapped Excitons and Energy Transfers in Vacancy‐Ordered Hexagonal Halide Perovskite Cs 2 HfF 6 Doped with Rare Earths for Radiation Detection. Germany: N. p., 2022.
Web. doi:10.1002/adom.202201374.
Adhikari, Menuka, Shrivastava, Navadeep, McClain, Starfari T., Adhikari, Chandra M., Guzelturk, Burak, Khanal, Rabi, Gautam, Bhoj, & Luo, Zhiping. Luminescence from Self‐Trapped Excitons and Energy Transfers in Vacancy‐Ordered Hexagonal Halide Perovskite Cs 2 HfF 6 Doped with Rare Earths for Radiation Detection. Germany. https://doi.org/10.1002/adom.202201374
Adhikari, Menuka, Shrivastava, Navadeep, McClain, Starfari T., Adhikari, Chandra M., Guzelturk, Burak, Khanal, Rabi, Gautam, Bhoj, and Luo, Zhiping. Mon .
"Luminescence from Self‐Trapped Excitons and Energy Transfers in Vacancy‐Ordered Hexagonal Halide Perovskite Cs 2 HfF 6 Doped with Rare Earths for Radiation Detection". Germany. https://doi.org/10.1002/adom.202201374.
@article{osti_1881541,
title = {Luminescence from Self‐Trapped Excitons and Energy Transfers in Vacancy‐Ordered Hexagonal Halide Perovskite Cs 2 HfF 6 Doped with Rare Earths for Radiation Detection},
author = {Adhikari, Menuka and Shrivastava, Navadeep and McClain, Starfari T. and Adhikari, Chandra M. and Guzelturk, Burak and Khanal, Rabi and Gautam, Bhoj and Luo, Zhiping},
abstractNote = {Compared to halides Cs2HfX6 (X = Cl, Br, I) with a vacancy-ordered cubic double perovskite structure, the halide Cs2HfF6 (CHF), with a hexagonal Bravais lattice, possesses a higher mass density and chemical stability for radiation detection. Luminescence properties and energy transfer mechanisms of rare-earths-doped CHF materials are studied here. The structure of CHF is identified as a new type of vacancy-ordered hexagonal perovskite, with the same type of building blocks of the double perovskite but stacked with single layers. Density-functional theory calculations reveal a large bandgap of CHF. A broad emission is observed from the pristine CHF host, which is suggested to be associated with self-trapped excitons (STEs). A series of rare-earths-doped materials are designed utilizing the STE emissions, and efficient energy transfers from STEs and Tb3+ to Eu3+ are achieved for tunable emissions. The codoped material shows stable emission under X-ray irradiation, with 10.2% reduction from its initial emission intensity, associated with possible structural evolution by radiation-induced deformation of the soft host. The radiation responses of singly and codoped materials are evaluated, and the codoped material is found to be more sensitive to the radiation energy than the singly doped or pristine CHF for radiation detection.},
doi = {10.1002/adom.202201374},
journal = {Advanced Optical Materials},
number = 19,
volume = 10,
place = {Germany},
year = {Mon Aug 15 00:00:00 EDT 2022},
month = {Mon Aug 15 00:00:00 EDT 2022}
}
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