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Journal Article

Atomic-Scale Observation of Irradiation-Induced Surface Oxidation by In Situ Transmission Electron Microscopy

MPS-Authors
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Huang,  Xing
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Jones,  Travis
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Fan,  Hua
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Willinger,  Marc Georg
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Citation

Huang, X., Jones, T., Fan, H., & Willinger, M. G. (2016). Atomic-Scale Observation of Irradiation-Induced Surface Oxidation by In Situ Transmission Electron Microscopy. Advanced Materials Interfaces, 3(22): 1600751. doi:10.1002/admi.201600751.


Cite as: https://hdl.handle.net/11858/00-001M-0000-002C-16A8-C
Abstract
Irradiation of materials with high energy particles can induce structural transitions or trigger chemical reactions. Understanding the underlying mechanism for irradiation-induced phenomena is of both scientific and technical importance. Here, CdS nanoribbons are used as a model system to study structural and chemical evolution under electron-beam irradiation by in situ transmission electron microscopy. Real-time imaging clearly shows that upon irradiation, CdS is transformed to CdO with the formation of orientation-dependent relationships at surface. The structural transition can always be triggered with a dose rate beyond 601 e/Å2s in this system. A lower dose rate instead leads to the deposition of an amorphous carbon layer on the surface. Based on real-time observations and density functional theory calculations, a mechanism for the oxidation of CdS to CdO is proposed. It is essentially a thermodynamically driven process that is mediated by the formation of sulfur vacancies due to the electron-beam irradiation. It is also demonstrated that the surface oxidation can be suppressed by pre-depositing a conductive carbon layer on the CdS surface. The carbon coating can effectively reduce the rate of sulfur vacancy creation, thus decreasing defect-mediated oxidation. In addition, it isolates the active oxygen radicals from the ribbon, blocking the pathway for oxygen diffusion.