Observations of grain-boundary phase transformations in an elemental metal

Meiners, Thorsten; Frolov, Timofey; Rudd, Robert E.; Dehm, Gerhard; Liebscher, Christian H.

doi:10.1038/s41586-020-2082-6

Title: Observations of grain-boundary phase transformations in an elemental metal

Journal Article · Wed Mar 18 00:00:00 EDT 2020 · Nature (London)

DOI:https://doi.org/10.1038/s41586-020-2082-6· OSTI ID:1872283

Meiners, Thorsten ^[1]; Frolov, Timofey ^[2]; Rudd, Robert E. ^[2];

^[1]; Liebscher, Christian H. ^[1]

Max-Planck-Institut für Eisenforschung, Düsseldorf (Germany)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

The theory of grain boundary (the interface between crystallites, GB) structure has a long history¹ and the concept of GBs undergoing phase transformations was proposed 50 years ago^2,3. The underlying assumption was that multiple stable and metastable states exist for different GB orientations^4,5,6. The terminology ‘complexion’ was recently proposed to distinguish between interfacial states that differ in any equilibrium thermodynamic property⁷. Different types of complexion and transitions between complexions have been characterized, mostly in binary or multicomponent systems^{8,9,10,11,12,13,14,15,16,17,18,19}. Simulations have provided insight into the phase behaviour of interfaces and shown that GB transitions can occur in many material systems^{20,21,22,23,24}. However, the direct experimental observation and transformation kinetics of GBs in an elemental metal have remained elusive. In this work we demonstrate atomic-scale GB phase coexistence and transformations at symmetric and asymmetric $$[11\bar{1}]$$ tilt GBs in elemental copper. Atomic-resolution imaging reveals the coexistence of two different structures at Σ19b GBs (where Σ19 is the density of coincident sites and b is a GB variant), in agreement with evolutionary GB structure search and clustering analysis^21,25,26. We also use finite-temperature molecular dynamics simulations to explore the coexistence and transformation kinetics of these GB phases. Our results demonstrate how GB phases can be kinetically trapped, enabling atomic-scale room-temperature observations. Our work paves the way for atomic-scale in situ studies of metallic GB phase transformations, which were previously detected only indirectly^{9,15,27,28,29}, through their influence on abnormal grain growth, non-Arrhenius-type diffusion or liquid metal embrittlement.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); European Research Council (ERC); USDOE Laboratory Directed Research and Development (LDRD) Program. Lawrence Livermore National Laboratory (LLNL)

Grant/Contract Number:: AC52-07NA27344; 787446

OSTI ID:: 1872283

Report Number(s):: LLNL-JRNL-791578; 990783

Journal Information:: Nature (London), Vol. 579, Issue 7799; ISSN 0028-0836

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (42)

Complexion: A new concept for kinetic engineering in materials science Dillon, Shen J.; Tang, Ming; Carter, W. Craig Acta Materialia, Vol. 55, Issue 18 https://doi.org/10.1016/j.actamat.2007.07.029	journal	October 2007
Small-scale plasticity in thin Cu and Al films Dehm, Gerhard; Balk, T. John; Edongué, Hervais Microelectronic Engineering, Vol. 70, Issue 2-4 https://doi.org/10.1016/S0167-9317(03)00395-2	journal	November 2003
Segregation-Induced Nanofaceting Transition at an Asymmetric Tilt Grain Boundary in Copper Peter, Nicolas J.; Frolov, Timofey; Duarte, Maria J. Physical Review Letters, Vol. 121, Issue 25 https://doi.org/10.1103/PhysRevLett.121.255502	journal	December 2018
Diffusion and segregation of silver in copper $Σ$ 5(310) grain boundary Divinski, Sergiy V.; Edelhoff, Henning; Prokofjev, Sergei Physical Review B, Vol. 85, Issue 14 https://doi.org/10.1103/PhysRevB.85.144104	journal	April 2012
Nonequilibrium free-energy calculation of solids using LAMMPS Freitas, Rodrigo; Asta, Mark; de Koning, Maurice Computational Materials Science, Vol. 112 https://doi.org/10.1016/j.commatsci.2015.10.050	journal	February 2016
Atom-resolved imaging of ordered defect superstructures at individual grain boundaries Wang, Zhongchang; Saito, Mitsuhiro; McKenna, Keith P. Nature, Vol. 479, Issue 7373 https://doi.org/10.1038/nature10593	journal	November 2011
The role of grain boundary energy in grain boundary complexion transitions Rohrer, Gregory S. Current Opinion in Solid State and Materials Science, Vol. 20, Issue 5 https://doi.org/10.1016/j.cossms.2016.03.001	journal	October 2016
Diffuse interface model for structural transitions of grain boundaries Tang, Ming; Carter, W. Craig; Cannon, Rowland M. Physical Review B, Vol. 73, Issue 2 https://doi.org/10.1103/PhysRevB.73.024102	journal	January 2006
New developments in evolutionary structure prediction algorithm USPEX Lyakhov, Andriy O.; Oganov, Artem R.; Stokes, Harold T. Computer Physics Communications, Vol. 184, Issue 4 https://doi.org/10.1016/j.cpc.2012.12.009	journal	April 2013
Transformation of ∑17 special tilt boundaries to general boundaries in tin Maksimova, E. L.; Shvindlerman, L. S.; Straumal, B. B. Acta Metallurgica, Vol. 36, Issue 6 https://doi.org/10.1016/0001-6160(88)90225-8	journal	June 1988
The Role of a Bilayer Interfacial Phase on Liquid Metal Embrittlement Luo, J.; Cheng, H.; Asl, K. M. Science, Vol. 333, Issue 6050 https://doi.org/10.1126/science.1208774	journal	September 2011
Evaluation of harmonic methods for calculating the free energy of defects in solids Foiles, Stephen M. Physical Review B, Vol. 49, Issue 21 https://doi.org/10.1103/PhysRevB.49.14930	journal	June 1994
A Streaming Multi-GPU Implementation of Image Simulation Algorithms for Scanning Transmission Electron Microscopy Pryor, Alan; Ophus, Colin; Miao, Jianwei arXiv https://doi.org/10.48550/arxiv.1706.08563	preprint	January 2017
Grain Boundary Transitions in Binary Alloys Tang, Ming; Carter, W. Craig; Cannon, Rowland M. Physical Review Letters, Vol. 97, Issue 7 https://doi.org/10.1103/PhysRevLett.97.075502	journal	August 2006
Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
Bismuth embrittlement of copper is an atomic size effect Schweinfest, Rainer; Paxton, Anthony T.; Finnis, Michael W. Nature, Vol. 432, Issue 7020 https://doi.org/10.1038/nature03198	journal	December 2004
Evidence for grain boundary phase transition in a 2d bicrystal Carrion, Francisco; Kalonji, Gretchen; Yip, Sidney Scripta Metallurgica, Vol. 17, Issue 7 https://doi.org/10.1016/0036-9748(83)90261-2	journal	July 1983
Grain boundary phases in bcc metals Frolov, T.; Setyawan, W.; Kurtz, R. J. Nanoscale, Vol. 10, Issue 17 https://doi.org/10.1039/C8NR00271A	journal	January 2018
Mechanically enhanced grain boundary structural phase transformation in Cu Aramfard, Mohammad; Deng, Chuang Acta Materialia, Vol. 146 https://doi.org/10.1016/j.actamat.2017.12.062	journal	March 2018
Visualization and analysis of atomistic simulation data with OVITO–the Open Visualization Tool Stukowski, Alexander Modelling and Simulation in Materials Science and Engineering, Vol. 18, Issue 1 https://doi.org/10.1088/0965-0393/18/1/015012	journal	December 2009
Nonequilibrium free-energy calculation of solids using LAMMPS Freitas, Rodrigo; Asta, Mark; de Koning, Maurice arXiv https://doi.org/10.48550/arxiv.2201.04622	text	January 2022
A genetic algorithm for predicting the structures of interfaces in multicomponent systems Chua, Alvin L. -S.; Benedek, Nicole A.; Chen, Lin Nature Materials, Vol. 9, Issue 5 https://doi.org/10.1038/nmat2712	journal	February 2010
A fast image simulation algorithm for scanning transmission electron microscopy Ophus, Colin Advanced Structural and Chemical Imaging, Vol. 3, Issue 1 https://doi.org/10.1186/s40679-017-0046-1	journal	May 2017
Grain Boundary Phase Transformations Hart, Edward W. The Nature and Behavior of Grain Boundaries https://doi.org/10.1007/978-1-4757-0181-4_6	book	January 1972
Congruent Phase Transition at a Twist Boundary Induced by Solute Segregation Udler, D.; Seidman, D. N. Physical Review Letters, Vol. 77, Issue 16 https://doi.org/10.1103/PhysRevLett.77.3379	journal	October 1996
Grain-boundary metastability and its statistical properties Han, Jian; Vitek, Vaclav; Srolovitz, David J. Acta Materialia, Vol. 104 https://doi.org/10.1016/j.actamat.2015.11.035	journal	February 2016
Grain boundary complexions in ceramics and metals: An overview Dillon, Shen J.; Harmer, Martin P.; Luo, Jian JOM, Vol. 61, Issue 12 https://doi.org/10.1007/s11837-009-0179-3	journal	December 2009
Grain boundary complexions in multicomponent alloys: Challenges and opportunities Zhou, Naixie; Hu, Tao; Luo, Jian Current Opinion in Solid State and Materials Science, Vol. 20, Issue 5 https://doi.org/10.1016/j.cossms.2016.05.001	journal	October 2016
Thermodynamics of coherent interfaces under mechanical stresses. I. Theory Frolov, T.; Mishin, Y. arXiv https://doi.org/10.48550/arxiv.1304.0144	text	January 2013
Structural phase transformations in metallic grain boundaries Frolov, Timofey; Olmsted, David L.; Asta, Mark Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms2919	journal	May 2013
A streaming multi-GPU implementation of image simulation algorithms for scanning transmission electron microscopy Pryor, Alan; Ophus, Colin; Miao, Jianwei Advanced Structural and Chemical Imaging, Vol. 3, Issue 1 https://doi.org/10.1186/s40679-017-0048-z	journal	October 2017
Two-dimensional phase transformation in grain boundaries Hart, Edward W. Scripta Metallurgica, Vol. 2, Issue 3 https://doi.org/10.1016/0036-9748(68)90222-6	journal	March 1968
Segregation-induced ordered superstructures at general grain boundaries in a nickel-bismuth alloy Yu, Zhiyang; Cantwell, Patrick R.; Gao, Qin Science, Vol. 358, Issue 6359 https://doi.org/10.1126/science.aam8256	journal	October 2017
X-ray microdiffraction: local stress distributions in polycrystalline and epitaxial thin films Phillips, M. A.; Spolenak, R.; Tamura, N. Microelectronic Engineering, Vol. 75, Issue 1 https://doi.org/10.1016/j.mee.2003.12.053	journal	July 2004
Grain boundary phases in bcc metals Frolov, T.; Setyawan, W.; Kurtz, R. J. arXiv https://doi.org/10.48550/arxiv.1711.06775	preprint	January 2017
Crystal structure prediction using ab initio evolutionary techniques: Principles and applications Oganov, Artem R.; Glass, Colin W. The Journal of Chemical Physics, Vol. 124, Issue 24 https://doi.org/10.1063/1.2210932	journal	June 2006
Bismuth-induced embrittlement of copper grain boundaries Duscher, Gerd; Chisholm, Matthew F.; Alber, Uwe Nature Materials, Vol. 3, Issue 9 https://doi.org/10.1038/nmat1191	journal	August 2004
Manipulating the interfacial structure of nanomaterials to achieve a unique combination of strength and ductility Khalajhedayati, Amirhossein; Pan, Zhiliang; Rupert, Timothy J. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms10802	journal	February 2016
Grain boundary complexions Cantwell, Patrick R.; Tang, Ming; Dillon, Shen J. Acta Materialia, Vol. 62 https://doi.org/10.1016/j.actamat.2013.07.037	journal	January 2014
Thermodynamics of coherent interfaces under mechanical stresses. I. Theory Frolov, T.; Mishin, Y. Physical Review B, Vol. 85, Issue 22 https://doi.org/10.1103/PhysRevB.85.224106	journal	June 2012
Theory of Phase Transitions at Internal Interfaces Rottman, C. Le Journal de Physique Colloques, Vol. 49, Issue C5 https://doi.org/10.1051/jphyscol:1988538	journal	October 1988
Evidence for structural multiplicity of the Σ = 3 incoherent twin boundary in Cu from grain-boundary diffusion measurements Rabkin, E.; Minkwitz, C.; Herzig, Chr. Philosophical Magazine Letters, Vol. 79, Issue 7 https://doi.org/10.1080/095008399177020	journal	July 1999

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Grain boundary segregation transitions and critical phenomena in binary regular solutions: A systematics of complexion diagrams with universal characters Zhou, Naixie; Hu, Chongze; Luo, Jian Acta Materialia, Vol. 221 https://doi.org/10.1016/j.actamat.2021.117375	journal	December 2021
Grain-Boundary Topological Phase Transitions Chen, Kongtao; Srolovitz, David J.; Han, Jian arXiv https://doi.org/10.48550/arxiv.2011.01475	text	January 2020
Discovery of Electrochemically Induced Grain Boundary Transitions Nie, Jiuyuan; Hu, Chongze; Yan, Qizhang arXiv https://doi.org/10.48550/arxiv.2012.15862	text	January 2020
Robotic fabrication of high-quality lamellae for aberration-corrected transmission electron microscopy Tsurusawa, Hideyo; Nakanishi, Nobuto; Kawano, Kayoko arXiv https://doi.org/10.48550/arxiv.2102.09698	preprint	January 2021

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