In-situ observation of phase separation during growth of Cs2LiLaBr6:Ce crystals using energy-resolved neutron imaging

Anton S. Tremsin; Didier Perrodin; Adrian S. Losko; Sven C. Vogel; Takenao Shinohara; Kenichi Oikawa; Jeff H. Peterson; Chang Zhang; Jeffrey J. Derby; Alexander M. Zlokapa; Gregory A. Bizarri; Edith D. Bourret

doi:10.1021/acs.cgd.7b01048

In-situ observation of phase separation during growth of Cs₂LiLaBr₆:Ce crystals using energy-resolved neutron imaging

Anton S. Tremsin, Didier Perrodin, Adrian S. Losko, Sven C. Vogel, Takenao Shinohara, Kenichi Oikawa, Jeff H. Peterson, Chang Zhang, Jeffrey J. Derby, Alexander M. Zlokapa, Gregory A. Bizarri, Edith D. Bourret

Chemical Engineering and Materials Science

Research output: Contribution to journal › Article › peer-review

19 Scopus citations

Abstract

In-situ imaging and characterization of Cs₂LiLaBr₆:Ce crystal growth are performed utilizing energyresolved neutron imaging. The unique capability of neutrons to penetrate the furnace and to provide direct information on the materials within the furnace is used to visualize the growth dynamics, location, and shape of the liquid/solid interface and to map the elemental composition. Nontrivial dynamics of phase separation within the liquid and solid phases were observed and investigated. Quantitative projected two-dimensional maps of Li concentrations were obtained with submillimeter spatial resolution delineating Li-rich and Li-depleted areas. Concurrent variations in Cs and Br concentrations were identified. Good transparency was obtained in part of the ingot where the liquid phase separation has reached steady state, suggesting that nonstoichiometric materials may be optimal for the original charge. The results demonstrate that energy-resolved neutron imaging and its associated modalities can provide unique information for the optimization of crystal growth conditions, in particular having the potential to accelerate scale-up from laboratory to commercial production by improving the yield and quality of single crystal materials.

Original language	English (US)
Pages (from-to)	6372-6381
Number of pages	10
Journal	Crystal Growth and Design
Volume	17
Issue number	12
DOIs	https://doi.org/10.1021/acs.cgd.7b01048
State	Published - Dec 6 2017

Bibliographical note

Funding Information:
The authors would like to acknowledge the beamtime allocated at the Lujan Neutron Scattering Center at Los Alamos National Laboratory and Materials and Life Sciences Facility at J-PARC. We also thank David Wilson (LBNL) for his valuable help with the experimental hardware. This work was supported by the U.S. Department of Energy/NNSA/DNN R&D and managed by Lawrence Berkeley National Laboratory under Contract No. AC02-05CH11231. We also would like to acknowledge the generous donations of Virtex FPGAs and the Vivado design suite by Xilinx Inc. of San Jose, California, through the Xilinx University Program.

Publisher Copyright:
© 2017 American Chemical Society.

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Tremsin, A. S., Perrodin, D., Losko, A. S., Vogel, S. C., Shinohara, T., Oikawa, K., Peterson, J. H., Zhang, C., Derby, J. J., Zlokapa, A. M., Bizarri, G. A., & Bourret, E. D. (2017). In-situ observation of phase separation during growth of Cs₂LiLaBr₆:Ce crystals using energy-resolved neutron imaging. Crystal Growth and Design, 17(12), 6372-6381. https://doi.org/10.1021/acs.cgd.7b01048

Tremsin, AS, Perrodin, D, Losko, AS, Vogel, SC, Shinohara, T, Oikawa, K, Peterson, JH, Zhang, C, Derby, JJ, Zlokapa, AM, Bizarri, GA & Bourret, ED 2017, 'In-situ observation of phase separation during growth of Cs₂LiLaBr₆:Ce crystals using energy-resolved neutron imaging', Crystal Growth and Design, vol. 17, no. 12, pp. 6372-6381. https://doi.org/10.1021/acs.cgd.7b01048

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title = "In-situ observation of phase separation during growth of Cs2LiLaBr6:Ce crystals using energy-resolved neutron imaging",

abstract = "In-situ imaging and characterization of Cs2LiLaBr6:Ce crystal growth are performed utilizing energyresolved neutron imaging. The unique capability of neutrons to penetrate the furnace and to provide direct information on the materials within the furnace is used to visualize the growth dynamics, location, and shape of the liquid/solid interface and to map the elemental composition. Nontrivial dynamics of phase separation within the liquid and solid phases were observed and investigated. Quantitative projected two-dimensional maps of Li concentrations were obtained with submillimeter spatial resolution delineating Li-rich and Li-depleted areas. Concurrent variations in Cs and Br concentrations were identified. Good transparency was obtained in part of the ingot where the liquid phase separation has reached steady state, suggesting that nonstoichiometric materials may be optimal for the original charge. The results demonstrate that energy-resolved neutron imaging and its associated modalities can provide unique information for the optimization of crystal growth conditions, in particular having the potential to accelerate scale-up from laboratory to commercial production by improving the yield and quality of single crystal materials.",

author = "Tremsin, {Anton S.} and Didier Perrodin and Losko, {Adrian S.} and Vogel, {Sven C.} and Takenao Shinohara and Kenichi Oikawa and Peterson, {Jeff H.} and Chang Zhang and Derby, {Jeffrey J.} and Zlokapa, {Alexander M.} and Bizarri, {Gregory A.} and Bourret, {Edith D.}",

note = "Funding Information: The authors would like to acknowledge the beamtime allocated at the Lujan Neutron Scattering Center at Los Alamos National Laboratory and Materials and Life Sciences Facility at J-PARC. We also thank David Wilson (LBNL) for his valuable help with the experimental hardware. This work was supported by the U.S. Department of Energy/NNSA/DNN R&D and managed by Lawrence Berkeley National Laboratory under Contract No. AC02-05CH11231. We also would like to acknowledge the generous donations of Virtex FPGAs and the Vivado design suite by Xilinx Inc. of San Jose, California, through the Xilinx University Program. Publisher Copyright: {\textcopyright} 2017 American Chemical Society.",

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AU - Perrodin, Didier

AU - Losko, Adrian S.

AU - Vogel, Sven C.

AU - Shinohara, Takenao

AU - Oikawa, Kenichi

AU - Peterson, Jeff H.

AU - Zhang, Chang

AU - Derby, Jeffrey J.

AU - Zlokapa, Alexander M.

AU - Bizarri, Gregory A.

AU - Bourret, Edith D.

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PY - 2017/12/6

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N2 - In-situ imaging and characterization of Cs2LiLaBr6:Ce crystal growth are performed utilizing energyresolved neutron imaging. The unique capability of neutrons to penetrate the furnace and to provide direct information on the materials within the furnace is used to visualize the growth dynamics, location, and shape of the liquid/solid interface and to map the elemental composition. Nontrivial dynamics of phase separation within the liquid and solid phases were observed and investigated. Quantitative projected two-dimensional maps of Li concentrations were obtained with submillimeter spatial resolution delineating Li-rich and Li-depleted areas. Concurrent variations in Cs and Br concentrations were identified. Good transparency was obtained in part of the ingot where the liquid phase separation has reached steady state, suggesting that nonstoichiometric materials may be optimal for the original charge. The results demonstrate that energy-resolved neutron imaging and its associated modalities can provide unique information for the optimization of crystal growth conditions, in particular having the potential to accelerate scale-up from laboratory to commercial production by improving the yield and quality of single crystal materials.

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