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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

Abstract

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 incrementalmore » advances that have, in the past, typically relied on empiricism, experience, and intuition.« less

Authors:
 [1];  [1];  [1];  [1];  [2];  [3];  [3];  [3]; ORCiD logo [4]; ORCiD logo [4]
  1. Univ. of Minnesota, Minneapolis, MN (United States)
  2. Univ. of California, Berkeley, CA (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA). Office of Defense Nuclear Nonproliferation R&D (NA-22); USDOE
OSTI Identifier:
1605133
Alternate Identifier(s):
OSTI ID: 1775936
Report Number(s):
LA-UR-19-32682
Journal ID: ISSN 0022-0248
Grant/Contract Number:  
89233218CNA000001; NA0002514; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Crystal Growth
Additional Journal Information:
Journal Volume: 536; Journal Issue: C; Journal ID: ISSN 0022-0248
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; A1. Computer simulation; A1. Heat transfer; A1. Segregation; A1. Neutron imaging; A2. Bridgman technique; B2. Scintillator materials

Citation Formats

Derby, Jeffrey J., Zhang, Chang, Seebeck, Jan, Peterson, Jeffrey H., Tremsin, Anton S., Perrodin, Didier, Bizarri, Gregory A., Bourret, Edith D., Losko, Adrian Simon, and Vogel, Sven C.. Computational modeling and neutron imaging to understand interface shape and solute segregation during the vertical gradient freeze growth of BaBrCl:Eu. United States: N. p., 2020. Web. https://doi.org/10.1016/j.jcrysgro.2020.125572.
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.. Computational modeling and neutron imaging to understand interface shape and solute segregation during the vertical gradient freeze growth of BaBrCl:Eu. United States. https://doi.org/10.1016/j.jcrysgro.2020.125572
Derby, Jeffrey J., Zhang, Chang, Seebeck, Jan, Peterson, Jeffrey H., Tremsin, Anton S., Perrodin, Didier, Bizarri, Gregory A., Bourret, Edith D., Losko, Adrian Simon, and Vogel, Sven C.. Thu . "Computational modeling and neutron imaging to understand interface shape and solute segregation during the vertical gradient freeze growth of BaBrCl:Eu". United States. https://doi.org/10.1016/j.jcrysgro.2020.125572. https://www.osti.gov/servlets/purl/1605133.
@article{osti_1605133,
title = {Computational modeling and neutron imaging to understand interface shape and solute segregation during the vertical gradient freeze growth of BaBrCl:Eu},
author = {Derby, Jeffrey J. and Zhang, Chang and Seebeck, Jan and Peterson, Jeffrey H. and Tremsin, Anton S. and Perrodin, Didier and Bizarri, Gregory A. and Bourret, Edith D. and Losko, Adrian Simon and Vogel, Sven C.},
abstractNote = {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.},
doi = {10.1016/j.jcrysgro.2020.125572},
journal = {Journal of Crystal Growth},
number = C,
volume = 536,
place = {United States},
year = {2020},
month = {2}
}

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Works referenced in this record:

Certain Physical Properties of Single Crystals of Tungsten, Antimony, Bismuth, Tellurium, Cadmium, Zinc, and Tin
journal, January 1925

  • Bridgman, P. W.
  • Proceedings of the American Academy of Arts and Sciences, Vol. 60, Issue 6
  • DOI: 10.2307/25130058

Eine Methode zur Herstellung einkristalliger Metalle
journal, December 1924

  • Obreimow, I.; Schubnikow, L.
  • Zeitschrift f�r Physik, Vol. 25, Issue 1
  • DOI: 10.1007/BF01327506

The Production of Large Single Crystals of Lithium Fluoride
journal, March 1936

  • Stockbarger, Donald C.
  • Review of Scientific Instruments, Vol. 7, Issue 3
  • DOI: 10.1063/1.1752094

Quantitative Analysis of Microsegregation in Silicon Grown by the Czochralski Method
journal, February 1976

  • Murgai, A.; Gatos, H. C.; Witt, A. F.
  • Journal of The Electrochemical Society, Vol. 123, Issue 2
  • DOI: 10.1149/1.2132791

Quantitative Analysis of the Effects of Destabilizing Vertical Thermal Gradients on Crystal Growth and Segregation: Ga‐Doped Ge
journal, March 1978

  • Kim, K. M.; Witt, A. F.; Lichtensteiger, M.
  • Journal of The Electrochemical Society, Vol. 125, Issue 3
  • DOI: 10.1149/1.2131477

The effect of fluctuating growth rates on segregation in crystals grown from the melt
journal, March 1980


Growth rate dependence of the interface distribution coefficient in the system Ge-Ga
journal, November 1982


Analysis of crystal growth characteristics in a conventional vertical Bridgman configuration
journal, March 1984


Lateral photovoltage scanning (LPS) method for the visualization of the solid–liquid interface of Si1−xGex single crystals
journal, April 2002


Photoluminescence of Cd1—xZnxTe Crystals Grown by High-Pressure Bridgman Technique
journal, August 1997


Anomalous segregation during electrodynamic gradient freeze growth of cadmium zinc telluride
journal, June 2011


Interface shapes during vertical bridgman growth of (Pb, Sn)Te crystals
journal, July 1990


Growth and interface study of 2in diameter CdZnTe by THM technique
journal, September 2010


Thermal fields in the bridgman-Stockbarger technique
journal, November 1985


Convection in the vertical Bridgman-Stockbarger technique
journal, June 1988


Growth and characterization of lead bromide crystals
journal, September 1992


A transparent multizone furnace for crystal growth and flow visualization
journal, September 1994


A Study on the Interface Control of Vertical Bridgman Crystal Growth Using a Transparent Multizone Furnace
journal, March 1996


Growth of benzil crystals by vertical dynamic gradient freeze technique in a transparent furnace
journal, September 1997


On-line control of solid–liquid interface by state feedback
journal, September 1999


Active control of interface shape during the crystal growth of lead bromide
journal, March 1999


Auxiliary optical heating for controlled crystal growth
journal, April 2002


Vibroconvective mixing applied to vertical Bridgman growth
journal, October 2003


Growth of 2,5-diphenyloxazole-doped naphthalene crystal by Bridgman method and its fluorescence studies
journal, April 2008


Heat transfer process during the crystallization of benzil grown by the Bridgman–Stockbarger method
journal, February 2011


Interface control by rotating submerged heater/baffle in vertical Bridgman configuration
journal, September 2018


Exploring growth conditions and Eu2+ concentration effects for KSr2I5:Eu scintillator crystals II: Ø 25 mm crystals
journal, February 2018


Crystal Growth and Scintillation Properties of Eu2+ doped Cs4CaI6 and Cs4SrI6
journal, March 2018


Crystal growth and scintillation performance of Cs2HfCl6 and Cs2HfCl4Br2
journal, February 2018


Observation of the melting-solidification processes of an Al crystal by synchrotron X-ray topography
journal, September 1985


A procedure to visualize the melt-solid interface in Bridgman grown germanium and lead tin telluride
journal, January 1986


In-situ observation of LEC GaAs solid-liquid interface with newly developed X-ray image processing system
journal, August 1986


In-situ observation of solid-liquid interface shape by X-ray radiography during silicon single crystal growth
journal, September 1988


Direct observation by X-ray radiography of convection of molten silicon in the Czochralski growth method
journal, May 1988


Direct observation by X-ray radiography of convection of boric oxide in the GaAs liquid encapsulated czochralski growth
journal, February 1989


Natural and forced convection of molten silicon during Czochralski single crystal growth
journal, February 1989


Flow instability of molten silicon in the Czochralski configuration
journal, April 1990


In-situ observation of impurity diffusion boundary layer in silicon Czochralski growth
journal, January 1990


In-situ monitoring of dopant concentration variation in a silicon melt during Czochralski growth
journal, July 1991


Double-beam x-ray radiography system for three-dimensional flow visualization of molten silicon convection
journal, October 1993


Crystal–melt interface shape and dislocations during the melting of silicon
journal, January 2003


Visualization of liquid-solid interface morphologies in gallium subject to natural convection
journal, July 1994


Radioscopic visualization of indium antimonide growth by the vertical Bridgman-Stockbarger technique
journal, February 1995


A novel vertical Bridgman-Stockbarger crystal growth system with visualization capability
journal, May 1995


A radioscopic technique to study convective fluid dynamics in opaque liquid metals
journal, July 1997


Visualization of convective solidification in a vertical layer of Eutectic Ga-In Melt
journal, December 1996

  • Koster, J. N.; Derebail, R.; Grötzbach, A.
  • Applied Physics A: Materials Science & Processing, Vol. 64, Issue 1
  • DOI: 10.1007/s003390050442

Visualization study of melting and solidification in convecting hypoeutectic Ga-In alloy
journal, August 1998


Directional Solidification and Melting of Eutectic GaIn
journal, November 1999


In situ diagnostics of the crystal-growth process through neutron imaging: application to scintillators
journal, April 2016

  • Tremsin, Anton S.; Makowska, Małgorzata G.; Perrodin, Didier
  • Journal of Applied Crystallography, Vol. 49, Issue 3
  • DOI: 10.1107/S1600576716004350

Optimization of high count rate event counting detector with Microchannel Plates and quad Timepix readout
journal, July 2015

  • Tremsin, A. S.; Vallerga, J. V.; McPhate, J. B.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 787
  • DOI: 10.1016/j.nima.2014.10.047

Structure and scintillation of Eu2+-activated BaBrCl and solid solutions in the BaCl2–BaBr2 system
journal, June 2013


In-Situ Observation of Phase Separation During Growth of Cs 2 LiLaBr 6 :Ce Crystals Using Energy-Resolved Neutron Imaging
journal, October 2017

  • Tremsin, Anton S.; Perrodin, Didier; Losko, Adrian S.
  • Crystal Growth & Design, Vol. 17, Issue 12
  • DOI: 10.1021/acs.cgd.7b01048

Crystal structure evolution of BaBrCl and BaBrCl:5%Eu up to 1073 K by neutron diffraction
journal, March 2018

  • Onken, Drew R.; Williams, Richard T.; Perrodin, Didier
  • Journal of Applied Crystallography, Vol. 51, Issue 2
  • DOI: 10.1107/S1600576718002807

The redistribution of solute atoms during the solidification of metals
journal, July 1953


The Distribution of Solute in Crystals Grown from the Melt. Part I. Theoretical
journal, November 1953

  • Burton, J. A.; Prim, R. C.; Slichter, W. P.
  • The Journal of Chemical Physics, Vol. 21, Issue 11
  • DOI: 10.1063/1.1698728

A Mathematical Analysis of Solute Redistribution During Solidification
journal, December 1955

  • Smith, V. G.; Tiller, W. A.; Rutter, J. W.
  • Canadian Journal of Physics, Vol. 33, Issue 12
  • DOI: 10.1139/p55-089

Theory of transport processes in single crystal growth from the melt
journal, June 1988


Constitutional supercooling surface roughening
journal, March 2004


Fluid dynamics in crystal growth: The good, the bad, and the ugly
journal, June 2016


Development of a new powerful computer code CrysVUN++ especially designed for fast simulation of bulk crystal growth processes
journal, March 1999


Process modeling of the industrial VGF growth process using the software package CrysVUN++
journal, April 2000


A new hybrid method for the global modeling of convection in CZ crystal growth configurations
journal, May 2007


Analysis of the growth of cadmium zinc telluride in an electrodynamic gradient freeze furnace via a self-consistent, multi-scale numerical model
journal, March 2005


Fixed-point convergence of modular, steady-state heat transfer models coupling multiple scales and phenomena for melt–crystal growth
journal, January 2006

  • Yeckel, Andrew; Pandy, Arun; Derby, Jeffrey J.
  • International Journal for Numerical Methods in Engineering, Vol. 67, Issue 12
  • DOI: 10.1002/nme.1685

An approximate block Newton method for coupled iterations of nonlinear solvers: Theory and conjugate heat transfer applications
journal, December 2009

  • Yeckel, Andrew; Lun, Lisa; Derby, Jeffrey J.
  • Journal of Computational Physics, Vol. 228, Issue 23
  • DOI: 10.1016/j.jcp.2009.08.003

Multi-scale crystal growth computations via an approximate block Newton method
journal, April 2010


Crystal growth and characterization of alkali-earth halide scintillators
journal, August 2012


Czochralski growth of the mixed halides BaBrCl and BaBrCl:Eu
journal, February 2016


The heat of Fusion of the Alkali Metal Halides
journal, February 1960

  • Dworkin, A. S.; Bredig, M. A.
  • The Journal of Physical Chemistry, Vol. 64, Issue 2
  • DOI: 10.1021/j100831a023

Thermal Conductivity of Eight Halide Crystals in the Temperature Range 220°K to 390°K
journal, August 1960

  • McCarthy, Kathryn A.; Ballard, Stanley S.
  • Journal of Applied Physics, Vol. 31, Issue 8
  • DOI: 10.1063/1.1735853

Control of interface shape in the vertical bridgman-stockbarger technique
journal, January 1974


An axial temperature profile curvature criterion for the engineering of convex crystal growth interfaces in Bridgman systems
journal, June 2017


Radial segregation induced by natural convection and melt/solid interface shape in vertical bridgman growth
journal, October 1983


Modeling the vertical Bridgman growth of cadmium zinc telluride II. Transient analysis of zinc segregation
journal, October 1995


On the effects of ampoule tilting during vertical Bridgman growth: three-dimensional computations via a massively parallel, finite element method
journal, September 1996


New Segregation Phenomena in Metals
journal, August 1951