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

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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.

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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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Data availability

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgments

We thank J. Caraccio, R. Sharma, D. Wiedeman, and R. Gaume at the University of Central Florida for specimen preparation and useful discussions associated with analyses. We also thank R. Golovchak at Austin Peay State University, T. Loretz at Computer Engineering Service, and R. Loretz at Nuclear Physics Consultant for useful discussions related to the irradiation-induced structural modifications and glass’ thermal behavior.

Funding

This work was supported by the Defense Threat Reduction Agency under Contract No. HDTRA 1-13-1-0001. Singapore University of Technology and Design acknowledges funding from the Ministry of Education ACRF Tier 2 Grant and the National Research Foundation Competitive Research Grant.

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Authors and Affiliations

  1. New York State College of Ceramics, Alfred University, Alfred, USA

    Myungkoo Kang & Patrick E. Lynch

  2. CREOL, College of Optics and Photonics, University of Central Florida, Orlando, USA

    Myungkoo Kang, Laura Sisken, Cesar Blanco, Claudia Goncalves, Chanelle Arias, Anna Zachariou, Anupama Yadav & Kathleen A. Richardson

  3. Engineering Product Development, Singapore University of Technology and Design, Singapore, Singapore

    Byoung-Uk Sohn & Dawn T. H. Tan

  4. Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, USA

    Qingyang Du, Danhao Ma, Ruturaj Pujari, Juejun Hu & Anuradha M. Agarwal

  5. Department of Materials Science and Engineering, University of Central Florida, Orlando, USA

    Jonathan Lee

  6. Department of Materials Science and Engineering, Clemson University, Clemson, USA

    Spencer Novak & Igor Luzinov

  7. Department of Physics and Astronomy, Ursinus College, Collegeville, USA

    Casey M. Schwarz

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  1. Myungkoo Kang
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Contributions

M.K. and K.A.R. conceived the project. C.B., C.G., and A.Y. fabricated samples. Q.D., D.M., and R.P. carried out gamma irradiation. M.K., B.-U.S., L.S., C.A., A.Z., P.E.L., and J.L. performed characterizations and analyses. S.N., C.M.S., I.L., J.H., A.M.A., and D.T.H.T. provided useful comments. M.K. drafted and supervised the manuscript. All authors have read and agreed to the published version of the manuscript.

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Kang, M., Sohn, BU., Du, Q. et al. Self-healing mechanisms for Ge–Sb–S chalcogenide glasses upon gamma irradiation. MRS Bulletin (2024). https://doi.org/10.1557/s43577-024-00693-x

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