Computational modeling and neutron imaging to understand interface shape and solute segregation during the vertical gradient freeze growth of BaBrCl:Eu

Derby, Jeffrey J.; Zhang, Chang; Seebeck, Jan; Peterson, Jeffrey H.; Tremsin, Anton S.; Perrodin, Didier; Bizarri, Gregory A.; Bourret, Edith D.; Losko, Adrian Simon; Vogel, Sven C.

doi:10.1016/j.jcrysgro.2020.125572

Title: Computational modeling and neutron imaging to understand interface shape and solute segregation during the vertical gradient freeze growth of BaBrCl:Eu

Journal Article · Thu Feb 27 00:00:00 EST 2020 · Journal of Crystal Growth

DOI:https://doi.org/10.1016/j.jcrysgro.2020.125572· OSTI ID:1605133

Derby, Jeffrey J. ^[1]; Zhang, Chang ^[1]; Seebeck, Jan ^[1]; Peterson, Jeffrey H. ^[1]; Tremsin, Anton S. ^[2]; Perrodin, Didier ^[3]; Bizarri, Gregory A. ^[3]; Bourret, Edith D. ^[3];

^[4];

^[4]

Univ. of Minnesota, Minneapolis, MN (United States)
Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

In this work we apply continuum models to analyze phase change, heat transfer, fluid flow, solute transport, and segregation in order to understand prior neutron imaging observations of the vertical gradient freeze growth of Eu-doped BaBrCl. The models provide a rigorous framework in which to understand the mechanisms that are responsible for the complicated evolution of interface shape and dopant distribution in the growth experiment. We explain how a transition in the solid/liquid interface shape from concave to convex is driven by changes in radial heat transfer caused by furnace design. We also provide a mechanistic explanation of how dynamic growth conditions and changes of the flow structure in the melt result in complicated segregation patterns in this system. A growth pause caused by controller lock-up is shown to result in a band of solute depletion in accordance with classical theory. However, changing flow patterns during growth result in a non-monotonic axial distribution of solute that cannot be explained by simple application of classical segregation models. We assert that the approach presented here, namely the use of rigorous models in conjunction advanced diagnostics, such as neutron imaging, provides an exciting path forward for process optimization and control, accelerating the incremental advances that have, in the past, typically relied on empiricism, experience, and intuition.

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Research Organization:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA). Office of Defense Nuclear Nonproliferation R&D (NA-22); USDOE

Grant/Contract Number:: 89233218CNA000001; NA0002514; AC02-05CH11231

OSTI ID:: 1605133

Alternate ID(s):: OSTI ID: 1775936

Report Number(s):: LA-UR-19-32682

Journal Information:: Journal of Crystal Growth, Vol. 536, Issue C; ISSN 0022-0248

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 2 works

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Title: Computational modeling and neutron imaging to understand interface shape and solute segregation during the vertical gradient freeze growth of BaBrCl:Eu

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