Unraveling Temperature-Induced Vacancy Clustering in Tungsten: From Direct Microscopy to Atomistic Insights via Data-Driven Bayesian Sampling

The evolution of the microstructure of materials is primarily governed by defect-mediated diffusion. Here, we examine the intriguing role played by vacancies in tungsten, a strategic metal for high-temperature fusion-energy systems. We address the existing apparent contradictions between experimenta...

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Main Authors: Anruo Zhong, Clovis Lapointe, Alexandra M. Goryaeva, Kazuto Arakawa, Manuel Athènes, Mihai-Cosmin Marinica
Format: Article
Language:English
Published: American Physical Society 2025-02-01
Series:PRX Energy
Online Access:http://doi.org/10.1103/PRXEnergy.4.013008
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author Anruo Zhong
Clovis Lapointe
Alexandra M. Goryaeva
Kazuto Arakawa
Manuel Athènes
Mihai-Cosmin Marinica
author_facet Anruo Zhong
Clovis Lapointe
Alexandra M. Goryaeva
Kazuto Arakawa
Manuel Athènes
Mihai-Cosmin Marinica
author_sort Anruo Zhong
collection DOAJ
description The evolution of the microstructure of materials is primarily governed by defect-mediated diffusion. Here, we examine the intriguing role played by vacancies in tungsten, a strategic metal for high-temperature fusion-energy systems. We address the existing apparent contradictions between experimental observations indicating the presence of voids and theoretical predictions of vacancy self-repulsion by employing both experimental and theoretical methods. We have designed a transmission-electron-microscopy experiment and developed a theoretical data-driven approach using the Bayesian adaptive biasing force method to investigate the finite-temperature properties of mono- and di-vacancies and characterize their relative stability via their formation free energies. Our investigation reveals that di-vacancies are energetically unfavorable at low temperatures but stabilize entropically as the temperature increases. This result is entirely consistent with experimental observations of the clustering of quenched-in vacancies in tungsten during reannealing treatments at intermediate temperatures. This work provides critical insights into the temperature-dependent stability of defects, bridging the gap between theoretical predictions and experimental observations, with significant implications for the design and optimization of high-temperature materials for fusion.
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spelling doaj-art-0a2cc553693c4a03bf24e768ba0f7b462025-08-20T03:12:23ZengAmerican Physical SocietyPRX Energy2768-56082025-02-014101300810.1103/PRXEnergy.4.013008Unraveling Temperature-Induced Vacancy Clustering in Tungsten: From Direct Microscopy to Atomistic Insights via Data-Driven Bayesian SamplingAnruo ZhongClovis LapointeAlexandra M. GoryaevaKazuto ArakawaManuel AthènesMihai-Cosmin MarinicaThe evolution of the microstructure of materials is primarily governed by defect-mediated diffusion. Here, we examine the intriguing role played by vacancies in tungsten, a strategic metal for high-temperature fusion-energy systems. We address the existing apparent contradictions between experimental observations indicating the presence of voids and theoretical predictions of vacancy self-repulsion by employing both experimental and theoretical methods. We have designed a transmission-electron-microscopy experiment and developed a theoretical data-driven approach using the Bayesian adaptive biasing force method to investigate the finite-temperature properties of mono- and di-vacancies and characterize their relative stability via their formation free energies. Our investigation reveals that di-vacancies are energetically unfavorable at low temperatures but stabilize entropically as the temperature increases. This result is entirely consistent with experimental observations of the clustering of quenched-in vacancies in tungsten during reannealing treatments at intermediate temperatures. This work provides critical insights into the temperature-dependent stability of defects, bridging the gap between theoretical predictions and experimental observations, with significant implications for the design and optimization of high-temperature materials for fusion.http://doi.org/10.1103/PRXEnergy.4.013008
spellingShingle Anruo Zhong
Clovis Lapointe
Alexandra M. Goryaeva
Kazuto Arakawa
Manuel Athènes
Mihai-Cosmin Marinica
Unraveling Temperature-Induced Vacancy Clustering in Tungsten: From Direct Microscopy to Atomistic Insights via Data-Driven Bayesian Sampling
PRX Energy
title Unraveling Temperature-Induced Vacancy Clustering in Tungsten: From Direct Microscopy to Atomistic Insights via Data-Driven Bayesian Sampling
title_full Unraveling Temperature-Induced Vacancy Clustering in Tungsten: From Direct Microscopy to Atomistic Insights via Data-Driven Bayesian Sampling
title_fullStr Unraveling Temperature-Induced Vacancy Clustering in Tungsten: From Direct Microscopy to Atomistic Insights via Data-Driven Bayesian Sampling
title_full_unstemmed Unraveling Temperature-Induced Vacancy Clustering in Tungsten: From Direct Microscopy to Atomistic Insights via Data-Driven Bayesian Sampling
title_short Unraveling Temperature-Induced Vacancy Clustering in Tungsten: From Direct Microscopy to Atomistic Insights via Data-Driven Bayesian Sampling
title_sort unraveling temperature induced vacancy clustering in tungsten from direct microscopy to atomistic insights via data driven bayesian sampling
url http://doi.org/10.1103/PRXEnergy.4.013008
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