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Uncovering Radiation Chemistry in the Solid State Through Periodic Density-Functional Calculations: Confrontation with Experimental Results and Beyond

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Applications of EPR in Radiation Research

Abstract

Three questions are crucial to unravel the radiation chemistry of any solid-state molecular system: what is the structure of the radicals formed, how are they formed and why? Molecular modeling methods based on Density Functional Theory—in confrontation with experimental Electron Paramagnetic Resonance (EPR) results—can help in finding an answer to all three questions. In this contribution, one view on how to perform such computational research is presented, with emphasis on the application of a periodic approach to biomolecules such as amino acids and carbohydrates. General strategies are outlined and common pitfalls are indicated. Topics include: effect of level of theory, model space and temperature on calculated EPR properties, formation mechanisms of radiation-induced radicals, and reaction path simulations for radiochemical transformations. In three case studies, these principles are applied to several radiation-induced radicals of sucrose.

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Acknowledgments

This work is supported by the Fund for Scientific Research—Flanders (FWO) and the Research Board of the Ghent University. All computational resources (Stevin Supercomputer Infrastructure) and services used in this work were provided by Ghent University, the Hercules Foundation and the Flemish Government—department EWI. This chapter is dedicated to children lost.

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  1. UGent HPC, Ghent University, Krijgslaan 281 S9, B-9000, Gent, Belgium

    Ewald Pauwels

  2. Center for Molecular Modeling, Ghent University, Technologiepark 903, B-9052, Zwijnaarde, Belgium

    Ewald Pauwels

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  1. Ewald Pauwels
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Correspondence to Ewald Pauwels .

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  1. The Emeritus Academy Linköping University, Linköping, Sweden

    Anders Lund

  2. Hiroshima University, Higashi-Hiroshima, Japan

    Masaru Shiotani

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Pauwels, E. (2014). Uncovering Radiation Chemistry in the Solid State Through Periodic Density-Functional Calculations: Confrontation with Experimental Results and Beyond. In: Lund, A., Shiotani, M. (eds) Applications of EPR in Radiation Research. Springer, Cham. https://doi.org/10.1007/978-3-319-09216-4_18

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