Grain boundary segregation in BCC vanadium-based alloys: Quantum-accurate computed segregation spectra and targeted experimental validations

Wagih, Malik; Lei, Tianjiao; Ng, Daniel; Schuh, Christopher A.

doi:10.1016/j.actamat.2025.121169

Grain boundary segregation in BCC vanadium-based alloys: Quantum-accurate computed segregation spectra and targeted experimental validations

Journal Article · Thu May 22 00:00:00 EDT 2025 · Acta Materialia

DOI:https://doi.org/10.1016/j.actamat.2025.121169· OSTI ID:2588637

^[1]; Lei, Tianjiao ^[2]; Ng, Daniel ^[3]; ^[4]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Univ. of Alabama, Tuscaloosa, AL (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Northwestern Univ., Evanston, IL (United States)

Grain boundaries are critically important to the material performance of fusion reactor materials such as vanadium, particularly mechanical properties and irradiation resistance. A key challenge to the design and control of grain boundaries in vanadium alloys is the lack of quantitative data on grain boundary segregation. In this study, we combine computational and experimental methods to address this gap. Furthermore, using a machine learning-accelerated quantum mechanics/molecular mechanics approach, we calculated the segregation spectra for 28 transition metal elements in polycrystalline vanadium, and validated these predictions experimentally for a subset of solutes that sample a range of segregation behavior, specifically zirconium, titanium, and tungsten, using analytical transmission electron microscopy. Furthermore, the agreement between experiment and theory highlights the predictive capability of our approach. Critically, this work provides a comprehensive database of quantum-accurate solute segregation enthalpies in vanadium, enabling the development of advanced alloys for fusion reactors applications.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 2588637

Report Number(s):: LLNL--JRNL-2002831

Journal Information:: Acta Materialia, Journal Name: Acta Materialia Vol. 294; ISSN 1359-6454

Publisher:: Elsevier BVCopyright Statement

Country of Publication:: United States

Language:: English

References (71)

Applications of the FIB lift-out technique for TEM specimen preparation Giannuzzi, Lucille A.; Drown, Jennifer L.; Brown, Steve R. Microscopy Research and Technique, Vol. 41, Issue 4 https://doi.org/10.1002/(SICI)1097-0029(19980515)41:4<285::AID-JEMT1>3.0.CO;2-Q	journal	May 1998
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
Anisotropy of segregation at grain boundaries and surfaces Wynblatt, Paul; Chatain, Dominique Metallurgical and Materials Transactions A, Vol. 37, Issue 9 https://doi.org/10.1007/BF02586096	journal	September 2006
The spectrum of binding energies approach to grain boundary segregation White, C. L.; Coghlan, W. A. Metallurgical Transactions A, Vol. 8, Issue 9 https://doi.org/10.1007/BF02642853	journal	September 1977
Sulfur segregation to grain boundaries in Ni3Al and Ni3(AI,Ti) alloys White, C. L.; Stein, D. F. Metallurgical Transactions A, Vol. 9, Issue 1 https://doi.org/10.1007/BF02647165	journal	January 1978
Grain growth and second-phase precipitation in nanocrystalline aluminum–manganese electrodeposits Huang, Ting-Yun; Kalidindi, Arvind R.; Schuh, Christopher A. Journal of Materials Science, Vol. 53, Issue 5 https://doi.org/10.1007/s10853-017-1764-4	journal	November 2017
Self-diffusion in body-centered cubic titanium-vanadium alloys Murdock, J. F.; McHargue, C. J. Acta Metallurgica, Vol. 16, Issue 4 https://doi.org/10.1016/0001-6160(68)90123-5	journal	April 1968
Radiation-induced segregation in binary and ternary alloys Okamoto, P. R.; Rehn, L. E. Journal of Nuclear Materials, Vol. 83, Issue 1 https://doi.org/10.1016/0022-3115(79)90587-7	journal	August 1979
Vanadium-base alloys for fusion reactor applications — a review Smith, D. L.; Loomis, B. A.; Diercks, D. R. Journal of Nuclear Materials, Vol. 135, Issue 2-3 https://doi.org/10.1016/0022-3115(85)90070-4	journal	October 1985
Alloying and impurity effects in vanadium-base alloys Diercks, D. R.; Loomis, B. A. Journal of Nuclear Materials, Vol. 141-143 https://doi.org/10.1016/0022-3115(86)90152-2	journal	November 1986
Void formation and precipitation in neutron irradiated vanadium alloys Ohnuki, S.; Takahashi, H.; Kinoshita, H. Journal of Nuclear Materials, Vol. 155-157 https://doi.org/10.1016/0022-3115(88)90444-8	journal	July 1988
Hydrogen solubility and diffusivity in defective and amorphous metals Kirchheim, R. Progress in Materials Science, Vol. 32, Issue 4 https://doi.org/10.1016/0079-6425(88)90010-2	journal	January 1988
Accurate ab initio energetics of extended systems via explicit correlation embedded in a density functional environment Govind, N.; Wang, Y. A.; da Silva, A. J. R. Chemical Physics Letters, Vol. 295, Issue 1-2 https://doi.org/10.1016/S0009-2614(98)00939-7	journal	October 1998
Vanadium alloys – overview and recent results Muroga, T.; Nagasaka, T.; Abe, K. Journal of Nuclear Materials, Vol. 307-311 https://doi.org/10.1016/S0022-3115(02)01253-9	journal	December 2002
Grain boundary chemistry and heat treatment effects on the ductile-to-brittle transition behavior of vanadium alloys Kurtz, R. J.; Hamilton, M. L.; Li, H. Journal of Nuclear Materials, Vol. 258-263 https://doi.org/10.1016/S0022-3115(98)00161-5	journal	October 1998
Grain boundary segregation of impurities in neutron irradiated and thermally aged vanadium alloys Kameda, J.; Bloomer, T. E.; Lyu, D. Y. Journal of Nuclear Materials, Vol. 258-263 https://doi.org/10.1016/S0022-3115(98)00174-3	journal	October 1998
Research and development on vanadium alloys for fusion applications Zinkle, S. J.; Matsui, H.; Smith, D. L. Journal of Nuclear Materials, Vol. 258-263 https://doi.org/10.1016/S0022-3115(98)00269-4	journal	October 1998
Stability of binary nanocrystalline alloys against grain growth and phase separation Murdoch, Heather A.; Schuh, Christopher A. Acta Materialia, Vol. 61, Issue 6 https://doi.org/10.1016/j.actamat.2012.12.033	journal	April 2013
Ab initio modelling of solute segregation energies to a general grain boundary Huber, Liam; Grabowski, Blazej; Militzer, Matthias Acta Materialia, Vol. 132 https://doi.org/10.1016/j.actamat.2017.04.024	journal	June 2017
Spectrum of grain boundary segregation energies in a polycrystal Wagih, Malik; Schuh, Christopher A. Acta Materialia, Vol. 181 https://doi.org/10.1016/j.actamat.2019.09.034	journal	December 2019
Role of grain boundary character and its evolution on interfacial solute segregation behavior in nanocrystalline Ni-P Gupta, Ankit; Zhou, Xuyang; Thompson, Gregory B. Acta Materialia, Vol. 190 https://doi.org/10.1016/j.actamat.2020.03.012	journal	May 2020
The vibrational entropy spectra of grain boundary segregation in polycrystals Tuchinda, Nutth; Schuh, Christopher A. Acta Materialia, Vol. 245 https://doi.org/10.1016/j.actamat.2022.118630	journal	February 2023
Atomistic simulations and machine learning of solute grain boundary segregation in Mg alloys at finite temperatures Menon, Vaidehi; Das, Sambit; Gavini, Vikram Acta Materialia, Vol. 264 https://doi.org/10.1016/j.actamat.2023.119515	journal	January 2024
Grain boundary segregation predicted by quantum-accurate segregation spectra but not by classical models Wagih, Malik; Naunheim, Yannick; Lei, Tianjiao Acta Materialia, Vol. 266 https://doi.org/10.1016/j.actamat.2024.119674	journal	March 2024
Grain boundary segregation for the Fe-P system: Insights from atomistic modeling and Bayesian inference Reichmann, Alexander; Tuchinda, Nutth; Dösinger, Christoph Acta Materialia, Vol. 279 https://doi.org/10.1016/j.actamat.2024.120215	journal	October 2024
A QM/MM approach for low-symmetry defects in metals Huber, Liam; Grabowski, Blazej; Militzer, Matthias Computational Materials Science, Vol. 118 https://doi.org/10.1016/j.commatsci.2016.03.028	journal	June 2016
Identifying interatomic potentials for the accurate modeling of interfacial segregation and structural transitions Hu, Yang; Schuler, Jennifer D.; Rupert, Timothy J. Computational Materials Science, Vol. 148 https://doi.org/10.1016/j.commatsci.2018.02.020	journal	June 2018
Computational modeling of grain boundary segregation: A review Hu, Chongze; Dingreville, Rémi; Boyce, Brad L. Computational Materials Science, Vol. 232 https://doi.org/10.1016/j.commatsci.2023.112596	journal	January 2024
Defects in magnesium and its alloys by atomistic simulation: Assessment of semi-empirical potentials Wang, Hexin; Guénolé, Julien; Korte-Kerzel, Sandra Computational Materials Science, Vol. 240 https://doi.org/10.1016/j.commatsci.2024.113025	journal	May 2024
Considerations for choosing and using force fields and interatomic potentials in materials science and engineering Becker, Chandler A.; Tavazza, Francesca; Trautt, Zachary T. Current Opinion in Solid State and Materials Science, Vol. 17, Issue 6 https://doi.org/10.1016/j.cossms.2013.10.001	journal	December 2013
Radiation-induced solute segregation in metallic alloys Ardell, Alan J.; Bellon, Pascal Current Opinion in Solid State and Materials Science, Vol. 20, Issue 3 https://doi.org/10.1016/j.cossms.2015.11.001	journal	June 2016
Implementing molecular dynamics on hybrid high performance computers – Particle–particle particle-mesh Brown, W. Michael; Kohlmeyer, Axel; Plimpton, Steven J. Computer Physics Communications, Vol. 183, Issue 3 https://doi.org/10.1016/j.cpc.2011.10.012	journal	March 2012
Atomsk: A tool for manipulating and converting atomic data files Hirel, Pierre Computer Physics Communications, Vol. 197 https://doi.org/10.1016/j.cpc.2015.07.012	journal	December 2015
LAMMPS - a flexible simulation tool for particle-based materials modeling at the atomic, meso, and continuum scales Thompson, Aidan P.; Aktulga, H. Metin; Berger, Richard Computer Physics Communications, Vol. 271 https://doi.org/10.1016/j.cpc.2021.108171	journal	February 2022
Recent progress on development of vanadium alloys for fusion Kurtz, R. J.; Abe, K.; Chernov, V. M. Journal of Nuclear Materials, Vol. 329-333 https://doi.org/10.1016/j.jnucmat.2004.04.299	journal	August 2004
Present status of vanadium alloys for fusion applications Muroga, T.; Chen, J. M.; Chernov, V. M. Journal of Nuclear Materials, Vol. 455, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2014.06.025	journal	December 2014
Effect of oxygen and nitrogen on microstructure and mechanical properties of vanadium Jo, Min-Gu; Madakashira, Phaniraj P.; Suh, Jin-Yu Materials Science and Engineering: A, Vol. 675 https://doi.org/10.1016/j.msea.2016.08.040	journal	October 2016
Automated inventory and material science scoping calculations under fission and fusion conditions Gilbert, Mark R.; Fleming, Michael; Sublet, Jean-Christophe Nuclear Engineering and Technology, Vol. 49, Issue 6 https://doi.org/10.1016/j.net.2017.07.005	journal	September 2017
Atomistic insights into the inhomogeneous nature of solute segregation to grain boundaries in magnesium Pei, Risheng; Xie, Zhuocheng; Yi, Sangbong Scripta Materialia, Vol. 230 https://doi.org/10.1016/j.scriptamat.2023.115432	journal	June 2023
The spectrum of interstitial solute energies in polycrystals Wagih, Malik; Schuh, Christopher A. Scripta Materialia, Vol. 235 https://doi.org/10.1016/j.scriptamat.2023.115631	journal	October 2023
Learning grain boundary segregation energy spectra in polycrystals Wagih, Malik; Larsen, Peter M.; Schuh, Christopher A. Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-20083-6	journal	December 2020
Aluminum depletion induced by co-segregation of carbon and boron in a bcc-iron grain boundary Ahmadian, A.; Scheiber, D.; Zhou, X. Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-26197-9	journal	October 2021
A machine learning approach to model solute grain boundary segregation Huber, Liam; Hadian, Raheleh; Grabowski, Blazej npj Computational Materials, Vol. 4, Issue 1 https://doi.org/10.1038/s41524-018-0122-7	journal	November 2018
Computed entropy spectra for grain boundary segregation in polycrystals Tuchinda, Nutth; Schuh, Christopher A. npj Computational Materials, Vol. 10, Issue 1 https://doi.org/10.1038/s41524-024-01260-3	journal	April 2024
Radiation-induced segregation in metals English, Colin A.; Murphy, Susan M.; Perks, Jonathan M. Journal of the Chemical Society, Faraday Transactions, Vol. 86, Issue 8 https://doi.org/10.1039/ft9908601263	journal	January 1990
Solute and solvent diffusion in V-Zr alloys Pruthi, D. D.; Agarwala, R. P. Philosophical Magazine A, Vol. 49, Issue 2 https://doi.org/10.1080/01418618408234927	journal	August 1984
Diffusion of 99Mo in vanadium Pelleg, Joshua; Zaklos, Y. Philosophical Magazine A, Vol. 63, Issue 3 https://doi.org/10.1080/01418619108213890	journal	March 1991
Hybrid atomistic simulation methods for materials systems Bernstein, N.; Kermode, J. R.; Csányi, G. Reports on Progress in Physics, Vol. 72, Issue 2 https://doi.org/10.1088/0034-4885/72/2/026501	journal	January 2009
Electronic structure calculations with GPAW: a real-space implementation of the projector augmented-wave method Enkovaara, J.; Rostgaard, C.; Mortensen, J. J. Journal of Physics: Condensed Matter, Vol. 22, Issue 25 https://doi.org/10.1088/0953-8984/22/25/253202	journal	June 2010
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
Structure identification methods for atomistic simulations of crystalline materials Stukowski, Alexander Modelling and Simulation in Materials Science and Engineering, Vol. 20, Issue 4 https://doi.org/10.1088/0965-0393/20/4/045021	journal	May 2012
The atomic simulation environment—a Python library for working with atoms Hjorth Larsen, Ask; Jørgen Mortensen, Jens; Blomqvist, Jakob Journal of Physics: Condensed Matter, Vol. 29, Issue 27 https://doi.org/10.1088/1361-648X/aa680e	journal	June 2017
Evaluating variability with atomistic simulations: the effect of potential and calculation methodology on the modeling of lattice and elastic constants Hale, Lucas M.; Trautt, Zachary T.; Becker, Chandler A. Modelling and Simulation in Materials Science and Engineering, Vol. 26, Issue 5 https://doi.org/10.1088/1361-651X/aabc05	journal	May 2018
Real-space grid implementation of the projector augmented wave method Mortensen, J. J.; Hansen, L. B.; Jacobsen, K. W. Physical Review B, Vol. 71, Issue 3 https://doi.org/10.1103/PhysRevB.71.035109	journal	January 2005
Multiscale simulations in simple metals: A density-functional-based methodology Choly, Nicholas; Lu, Gang; E., Weinan Physical Review B, Vol. 71, Issue 9 https://doi.org/10.1103/PhysRevB.71.094101	journal	March 2005
Simulation of the interaction between Fe impurities and point defects in V Mendelev, Mikhail I.; Han, Seungwu; Son, Won-joon Physical Review B, Vol. 76, Issue 21 https://doi.org/10.1103/PhysRevB.76.214105	journal	December 2007
Localized atomic basis set in the projector augmented wave method Larsen, A. H.; Vanin, M.; Mortensen, J. J. Physical Review B, Vol. 80, Issue 19 https://doi.org/10.1103/PhysRevB.80.195112	journal	November 2009
On representing chemical environments Bartók, Albert P.; Kondor, Risi; Csányi, Gábor Physical Review B, Vol. 87, Issue 18 https://doi.org/10.1103/PhysRevB.87.184115	journal	May 2013
Computing energy barriers for rare events from hybrid quantum/classical simulations through the virtual work principle Swinburne, Thomas D.; Kermode, James R. Physical Review B, Vol. 96, Issue 14 https://doi.org/10.1103/PhysRevB.96.144102	journal	October 2017
Gaussian Approximation Potentials: The Accuracy of Quantum Mechanics, without the Electrons Bartók, Albert P.; Payne, Mike C.; Kondor, Risi Physical Review Letters, Vol. 104, Issue 13 https://doi.org/10.1103/PhysRevLett.104.136403	journal	April 2010
Learning Grain-Boundary Segregation: From First Principles to Polycrystals Wagih, Malik; Schuh, Christopher A. Physical Review Letters, Vol. 129, Issue 4 https://doi.org/10.1103/PhysRevLett.129.046102	journal	July 2022
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Thermal Contraction and Disordering of the Al(110) Surface Marzari, Nicola; Vanderbilt, David; De Vita, Alessandro Physical Review Letters, Vol. 82, Issue 16 https://doi.org/10.1103/PhysRevLett.82.3296	journal	April 1999
Structural Relaxation Made Simple Bitzek, Erik; Koskinen, Pekka; Gähler, Franz Physical Review Letters, Vol. 97, Issue 17 https://doi.org/10.1103/PhysRevLett.97.170201	journal	October 2006
Least squares quantization in PCM Lloyd, S. IEEE Transactions on Information Theory, Vol. 28, Issue 2 https://doi.org/10.1109/TIT.1982.1056489	journal	March 1982
Probabilistic Principal Component Analysis Tipping, Michael E.; Bishop, Christopher M. Journal of the Royal Statistical Society: Series B (Statistical Methodology), Vol. 61, Issue 3, p. 611-622 https://doi.org/10.1111/1467-9868.00196	journal	August 1999
Subnanoscale Studies of Segregation at Grain Boundaries: Simulations and Experiments Seidman, David N. Annual Review of Materials Research, Vol. 32, Issue 1 https://doi.org/10.1146/annurev.matsci.32.011602.095455	journal	August 2002
Mechanical properties of vanadium and vanadium-base alloys Harrod, D. L.; Gold, R. E. International Materials Reviews, Vol. 25, Issue 1 https://doi.org/10.1179/095066080790136244	journal	January 1980
Swelling and Microstructural Changes in Irradiated Vanadium Alloys Bentley, J.; Wiffen, F. W. Nuclear Technology, Vol. 30, Issue 3 https://doi.org/10.13182/NT76-A31651	journal	September 1976
Estimation of grain boundary segregation enthalpy and its role in stable nanocrystalline alloy design Murdoch, Heather A.; Schuh, Christopher A. Journal of Materials Research, Vol. 28, Issue 16 https://doi.org/10.1557/jmr.2013.211	journal	August 2013
Atomistic Assessment of Solute-Solute Interactions during Grain Boundary Segregation Matson, Thomas P.; Schuh, Christopher A. Nanomaterials, Vol. 11, Issue 9 https://doi.org/10.3390/nano11092360	journal	September 2021

Similar Records

Grain boundary segregation of phosphorus in iron-vanadium alloys

Journal Article · Thu Oct 31 23:00:00 EST 1996 · Acta Materialia · OSTI ID:415425

Estimation of grain boundary segregation enthalpy and its role in stable nanocrystalline alloy design

Journal Article · Mon Aug 05 20:00:00 EDT 2013 · Journal of Materials Research · OSTI ID:1386990

Multiscale Modeling of Grain Boundary Segregation and Embrittlement in Tungsten for Mechanistic Design of Alloys for Coal Fired Plants

Technical Report · Sun Sep 29 00:00:00 EDT 2013 · OSTI ID:1096566

Related Subjects

Fusion materials
Grain boundary
Solute segregation
Thermodynamics
Vanadium alloys

Grain boundary segregation in BCC vanadium-based alloys: Quantum-accurate computed segregation spectra and targeted experimental validations

Citation Formats

References (71)

Similar Records

Related Subjects