In-situ observation and analysis of solid-state diffusion and liquid migration in a crystal growth system: A segregation-driven diffusion couple

Anton S. Tremsin, Didier Perrodin, Adrian S. Losko, Sven C. Vogel, Takenao Shinohara, Kenichi Oikawa, Gregory A. Bizarri, Edith D. Bourret, Jeffrey H. Peterson, Kerry P. Wang, Jeffrey J. Derby

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

Energy-resolved neutron imaging is employed for in-situ measurements of dopant transport in a simple experiment performed before the crystal growth of the scintillator BaBrCl:5%Eu via a vertical gradient freeze technique. During a stabilization period preceding growth, we observed the diffusion of Eu from the solid phase into the melt over a period of approximately 4 h. Comparing the measured centerline concentration profile with a mathematical model for the system, we estimate the solid-state diffusivity of Eu in BaBrCl as D1=1.9×10−10 m2/s and an upper limit for the liquid-phase diffusivity of Eu in the melt as D2 *=2.5×10−10 m2/s, at temperatures near the melting point. We compare this experiment, where diffusion is driven by a concentration discontinuity arising from segregation, to the classical diffusion couple technique. Suggestions are offered on how this segregation-driven couple might be improved as a tool for measuring diffusion coefficients, and we draw attention to the great promise of neutron imaging for in-situ measurements of the distribution of elements, with sufficiently high neutron attenuation coefficients, in difficult environments.

Original languageEnglish (US)
Pages (from-to)434-442
Number of pages9
JournalActa Materialia
Volume186
DOIs
StatePublished - Mar 2020

Bibliographical note

Funding Information:
The authors would like to acknowledge the generous donation of Vertex FPGA, Vivado design suite and a connectivity kit by Xilinx Inc. of San Jose, CA, through their Xilinx University Program. The detector used in these experiments was developed by the University of California at Berkeley in collaboration with Nova Scientific, and its readout was developed within the Medipix collaboration. 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 . The authors are also thankful to Czech Technical University in Prague, Advacam (Finland and Czech Republic), and NiKHEF (Netherlands) for the invaluable help with data acquisition hardware and software. The neutron experiment at the Materials and Life Science Experimental Facility of the J-PARC was performed under the user program (Proposal No. 2016B0183, 2017B0113, 2018A0038). The University of Minnesota effort was also supported in part by the U.S. Department of Energy Award DE-NA0002514 . No official endorsement should be inferred.

Funding Information:
The authors would like to acknowledge the generous donation of Vertex FPGA, Vivado design suite and a connectivity kit by Xilinx Inc. of San Jose, CA, through their Xilinx University Program. The detector used in these experiments was developed by the University of California at Berkeley in collaboration with Nova Scientific, and its readout was developed within the Medipix collaboration. 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. The authors are also thankful to Czech Technical University in Prague, Advacam (Finland and Czech Republic), and NiKHEF (Netherlands) for the invaluable help with data acquisition hardware and software. The neutron experiment at the Materials and Life Science Experimental Facility of the J-PARC was performed under the user program (Proposal No. 2016B0183, 2017B0113, 2018A0038). The University of Minnesota effort was also supported in part by the U.S. Department of Energy Award DE-NA0002514. No official endorsement should be inferred.

Publisher Copyright:
© 2020 Acta Materialia Inc.

Keywords

  • Diffusion
  • Modeling
  • Neutron imaging
  • Segregation
  • Solid/liquid interface

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