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Title: Improved Lithium Iodide neutron scintillator with Eu 2 + activation II: Activator zoning and concentration effects in Bridgman-grown crystals

Abstract

We have previously reported on the formation of Suzuki Phase precipitate particles as a result of the addition of the divalent activator ion Eu2+ to the monovalent alkali halide host LiI. [Boatner et al. (2017)]. These precipitates form during Bridgman or other melt-growth processes, even at low Eu2+ concentrations (e.g., 0.1% EuI2 doping), and scatter the scintillation light reducing the optical transparency of the scintillator and adversely affecting its radiation-detection performance. In our prior work, we developed a two-stage thermal-treatment method for the post-growth removal of the Suzuki Phase particles and the realization of a significant improvement in the optical transparency and associated neutron-detection of LiI:Eu2+ scintillators. These improvements resulted in neutron-detection performance that is superior to GS-20 glass and that allows for the application of pulse height gamma-ray discrimination over a wide range of gamma ray energies as opposed to pulse shape discrimination. Here in this paper, we apply the two-stage thermal-processing method for the removal of Suzuki phase precipitates and carry out an in-depth study, first, of the neutron scintillator performance versus the Eu2+ activator-ion-concentration spatial variation as a result of zoning effects during the Bridgman growth of LiI:Eu and, second, of the effects of varying the initialmore » Eu2+ activator ion concentration prior to crystal growth. The Eu2+ zoning variation results allow one to identify and select the most efficient location of the scintillation performance in a directionally solidified single-crystal boule. The present study of the initial activator concentration levels shows that there are, in fact, two distinct types of luminescence centers with varying performance properties — one that occurs only at low EuI2 addition levels (e.g., 0.01 to 0.06 %EuI2) and that is quickly replaced by a second luminescing center with increasing Eu content (e.g., at 0.1% EuI2). The light yield for the luminescing center formed using a Eu activator in LiI is a critical function of the Eu concentration in the range of 0.01 to 0.1 % EuI2, and a high light yield of 100,000 photons/neutron is observed at the 0.06 %EuIadditive level prior to thermal processing.« less

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [1];  [4];  [1]; ORCiD logo [1]
+ Show Author Affiliations
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology; Univ. of Tennessee, Knoxville, TN (United States). Nuclear Engineering Department and Scintillation Materials Research Center
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Nuclear Security and Isotope Technology Division
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Instrument and Source Division, Neutron Sciences Directorate
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation
OSTI Identifier:
1470866
Alternate Identifier(s):
OSTI ID: 1495637
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Nuclear Instruments and Methods in Physics Research. Section A, Accelerators, Spectrometers, Detectors and Associated Equipment
Additional Journal Information:
Journal Volume: 903; Journal Issue: C; Journal ID: ISSN 0168-9002
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Neutron detection; Scintillator crystals; Crystal growth; Suzuki Phase; Europium activator

Citation Formats

Boatner, Lynn A., Comer, Eleanor P., Wright, Gomez W., Ramey, Joanne Oxendine, Riedel, Richard A., Jellison Jr, Gerald Earle, and Kolopus, James A. Improved Lithium Iodide neutron scintillator with Eu 2+ activation II: Activator zoning and concentration effects in Bridgman-grown crystals. United States: N. p., 2018. Web. doi:10.1016/j.nima.2018.06.057.
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Boatner, Lynn A., Comer, Eleanor P., Wright, Gomez W., Ramey, Joanne Oxendine, Riedel, Richard A., Jellison Jr, Gerald Earle, & Kolopus, James A. Improved Lithium Iodide neutron scintillator with Eu 2+ activation II: Activator zoning and concentration effects in Bridgman-grown crystals. United States. https://doi.org/10.1016/j.nima.2018.06.057
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Boatner, Lynn A., Comer, Eleanor P., Wright, Gomez W., Ramey, Joanne Oxendine, Riedel, Richard A., Jellison Jr, Gerald Earle, and Kolopus, James A. Sat . "Improved Lithium Iodide neutron scintillator with Eu 2+ activation II: Activator zoning and concentration effects in Bridgman-grown crystals". United States. https://doi.org/10.1016/j.nima.2018.06.057. https://www.osti.gov/servlets/purl/1470866.
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@article{osti_1470866,
title = {Improved Lithium Iodide neutron scintillator with Eu 2+ activation II: Activator zoning and concentration effects in Bridgman-grown crystals},
author = {Boatner, Lynn A. and Comer, Eleanor P. and Wright, Gomez W. and Ramey, Joanne Oxendine and Riedel, Richard A. and Jellison Jr, Gerald Earle and Kolopus, James A.},
abstractNote = {We have previously reported on the formation of Suzuki Phase precipitate particles as a result of the addition of the divalent activator ion Eu2+ to the monovalent alkali halide host LiI. [Boatner et al. (2017)]. These precipitates form during Bridgman or other melt-growth processes, even at low Eu2+ concentrations (e.g., 0.1% EuI2 doping), and scatter the scintillation light reducing the optical transparency of the scintillator and adversely affecting its radiation-detection performance. In our prior work, we developed a two-stage thermal-treatment method for the post-growth removal of the Suzuki Phase particles and the realization of a significant improvement in the optical transparency and associated neutron-detection of LiI:Eu2+ scintillators. These improvements resulted in neutron-detection performance that is superior to GS-20 glass and that allows for the application of pulse height gamma-ray discrimination over a wide range of gamma ray energies as opposed to pulse shape discrimination. Here in this paper, we apply the two-stage thermal-processing method for the removal of Suzuki phase precipitates and carry out an in-depth study, first, of the neutron scintillator performance versus the Eu2+ activator-ion-concentration spatial variation as a result of zoning effects during the Bridgman growth of LiI:Eu and, second, of the effects of varying the initial Eu2+ activator ion concentration prior to crystal growth. The Eu2+ zoning variation results allow one to identify and select the most efficient location of the scintillation performance in a directionally solidified single-crystal boule. The present study of the initial activator concentration levels shows that there are, in fact, two distinct types of luminescence centers with varying performance properties — one that occurs only at low EuI2 addition levels (e.g., 0.01 to 0.06 %EuI2) and that is quickly replaced by a second luminescing center with increasing Eu content (e.g., at 0.1% EuI2). The light yield for the luminescing center formed using a Eu activator in LiI is a critical function of the Eu concentration in the range of 0.01 to 0.1 % EuI2, and a high light yield of 100,000 photons/neutron is observed at the 0.06 %EuIadditive level prior to thermal processing.},
doi = {10.1016/j.nima.2018.06.057},
journal = {Nuclear Instruments and Methods in Physics Research. Section A, Accelerators, Spectrometers, Detectors and Associated Equipment},
number = C,
volume = 903,
place = {United States},
year = {2018},
month = {9}
}
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https://doi.org/10.1016/j.nima.2018.06.057
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Works referenced in this record:

Improved lithium iodide neutron scintillator with Eu2+ activation: The elimination of Suzuki-Phase precipitates
journal, May 2017

  • Boatner, L. A.; Comer, E. P.; Wright, G. W.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 854
  • DOI: 10.1016/j.nima.2017.02.059

X-ray Studies on the Structures of Solid Solutions NaCl-CaCl 2 II. Structures of {111} and {310} Plate-Zones
journal, September 1955

  • Suzuki, Kazuo
  • Journal of the Physical Society of Japan, Vol. 10, Issue 9, p. 794-804
  • DOI: 10.1143/JPSJ.10.794

X-ray Studies on Precipitation of Metastable Centers in Mixed Crystals NaCl-CdCl 2
journal, January 1961

  • Suzuki, Kazuo
  • Journal of the Physical Society of Japan, Vol. 16, Issue 1, p. 67-78
  • DOI: 10.1143/JPSJ.16.67

Carbon coating of fused silica ampoules
journal, May 2006

Some lithium iodide phosphors for slow neutron detection
journal, March 1955

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    Works referencing / citing this record:

    Defect chemistry of Eu dopants in NaI scintillators studied by atomically resolved force microscopy
    journal, July 2019

    Critical Review of Scintillating Crystals for Neutron Detection
    journal, September 2019

    • Cieślak, Michał; Gamage, Kelum; Glover, Robert
    • Crystals, Vol. 9, Issue 9
    • DOI: 10.3390/cryst9090480
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