伽马辐照下 Ge-Sb-S 卤化物玻璃的自修复机制

IF 4.1 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY
Myungkoo Kang, Byoung-Uk Sohn, Qingyang Du, Danhao Ma, Ruturaj Pujari, Laura Sisken, Cesar Blanco, Claudia Goncalves, Chanelle Arias, Anna Zachariou, Anupama Yadav, Patrick E. Lynch, Jonathan Lee, Spencer Novak, Casey M. Schwarz, Igor Luzinov, Juejun Hu, Anuradha M. Agarwal, Dawn T. H. Tan, Kathleen A. Richardson
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引用次数: 0

摘要

摘要 我们报告了原子论机制,该机制将块状 Ge23Sb7S70 卤化物玻璃随时间变化的光学响应与其在伽马辐照后产生并随后湮灭的陨变结构缺陷直接联系起来。这些缺陷的特征是辐照引起的边缘共享 GeS4/2 四面体成键单元浓度的增加,在恢复过程中逐渐降低到辐照前的水平,从而说明了玻璃的陨变行为。这种随时间变化的结构变化导致了玻璃质量密度的演变,相应地引起了线性折射率和带隙能的变化和松弛。在线性光学特性发生变化的同时,我们发现玻璃的非线性响应没有受到影响,这可能是由于玻璃网络的自由电子产生了反作用。这些缺陷在伽马射线照射下产生,随后在室温下发生弛豫。我们研究的新颖之处在于,对这种关键的红外共卤玻璃进行了多方面的监测,包括光学、电子学、形态学、化学和微观结构特性,并将其与伽马射线辐照后的时间函数相互关联,以确定与未受辐照材料相比,材料系统行为背后的起源。据我们所知,这是首次采用综合方法(总结同一样品辐照前和辐照后的特性)来研究这一现象。可蜕变的块状掺杂玻璃中的行为是一个关键的基石,它将使材料系统能够作为稳健、可逆的辐射传感器部署在极端环境中,如伽马射线非常丰富的太空和地面放射性设施。我们论文中的发现可能会揭示钙化玻璃自愈合过程背后的微观起源这一悬而未决的问题。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Self-healing mechanisms for Ge–Sb–S chalcogenide glasses upon gamma irradiation

Self-healing mechanisms for Ge–Sb–S chalcogenide glasses upon gamma irradiation

Abstract

We report atomistic mechanisms that directly correlate the time-dependent optical responses of bulk Ge23Sb7S70 chalcogenide glasses to their metastable structural defects created and subsequently annihilated following gamma irradiation. These defects are characterized by an irradiation-induced increase in the concentration of edge-shared GeS4/2 tetrahedra bonding units, which gradually decreases to a pre-irradiation level during recovery, thus illustrating the glass’ metastable behavior. This time-dependent structural change gives rise to the evolution of the glass’s mass density that correspondingly induces a change and subsequent relaxation of linear refractive index and bandgap energy. Concurrent with this evolution in linear optical properties, the glass’ nonlinear response is found to be unaffected, likely due to a counter effect associated with the glass network’s free electrons.

Graphical abstract

Impact statement

Our work is the first study to employ a combined theoretical-experimental approach to the quantitative processing–structure–property relationship correlating the time-dependent structural and linear/nonlinear optical responses of chalcogenide Ge–Sb–S bulk glasses to their metastable topological coordination defects. These defects are created upon gamma-ray exposure and subsequently undergo relaxation at room temperature. The novelty of our study is that multifaceted aspects of such a key infrared chalcogenide glass, including optical, electronic, morphological, chemical, and microstructural properties, were monitored and cross-correlated as a function of time following gamma irradiation in order to identify origins behind the material system’s behavior as compared to base unirradiated material. This is, to our knowledge, the first-ever integrated approach (summarizing pre- and postexposure properties on the same samples) to the phenomenon. The behavior in metastable bulk chalcogenide glasses serves as a key cornerstone that will enable the material system to be deployed as robust, reversible radiation sensors in extreme environments such as space and ground-based radioactive facilities where gamma ray is characteristically abundant. Findings in our paper may shed light on the lingering question on the microscopic origin behind the self-healing process in chalcogenide glasses.

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来源期刊
Mrs Bulletin
Mrs Bulletin 工程技术-材料科学:综合
CiteScore
7.40
自引率
2.00%
发文量
193
审稿时长
4-8 weeks
期刊介绍: MRS Bulletin is one of the most widely recognized and highly respected publications in advanced materials research. Each month, the Bulletin provides a comprehensive overview of a specific materials theme, along with industry and policy developments, and MRS and materials-community news and events. Written by leading experts, the overview articles are useful references for specialists, but are also presented at a level understandable to a broad scientific audience.
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