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Thermodynamic and magnetic properties of surface Fe3+ species on quartz: effects of gamma-ray irradiation and implications for aerosol–radiation interactions

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Abstract

Samples of a natural amethyst, pulverized in air, and irradiated for gamma-ray doses from 0.14 to 70 kGy, have been investigated by powder electron paramagnetic resonance (EPR) spectroscopy from 90 to 294 K. The powder EPR spectra show that the surface Fe3+ species on the gamma-ray-irradiated quartz differ from its counterpart without irradiation in both the effective g value and the observed line shape, suggesting marked radiation effects. This suggestion is supported by quantitatively determined thermodynamic properties, magnetic susceptibility, relaxation times, and geometrical radius. In particular, the surface Fe3+ species on gamma-ray-irradiated quartz has larger Gibbs and activation energies than its non-irradiated counterpart, suggesting radiation-induced chemical reactions. The shorter phase-memory time (T m) but longer spin–lattice relaxation time (T 1) of the surface Fe3+ species on the gamma-ray-irradiated quartz than that without irradiation indicate stronger dipolar interactions in the former. Moreover, the calculated geometrical radius of the surface Fe3+ species on the gamma-ray-irradiated quartz is three orders of magnitude larger than that of its counterpart on the as-is sample. These results provide new insights into radiation-induced aerosol nucleation, with relevance to atmospheric cloud formation and global climate changes.

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Acknowledgments

We thank Dr. Milan Rieder for his suggestion of the experiments reported in Fig. 1, which was the impetus to this study. We also thank Dr. F. Di Benedetto and an anonymous reviewer for incisive criticisms and helpful suggestions, Drs. Kuppala V Narasimhulu and J. Lakshmana Rao for discussions, and the Natural Science and Engineering Research Council (NSERC) of Canada for financial support.

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Authors and Affiliations

  1. Department of Geological Sciences, University of Saskatchewan, Saskatoon, SK, S7N 5E2, Canada

    Gobburu SivaRamaiah & Yuanming Pan

  2. Department of Physics, Government College for Men, Kadapa, 516004, India

    Gobburu SivaRamaiah

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  1. Gobburu SivaRamaiah
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  2. Yuanming Pan
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Correspondence to Yuanming Pan.

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SivaRamaiah, G., Pan, Y. Thermodynamic and magnetic properties of surface Fe3+ species on quartz: effects of gamma-ray irradiation and implications for aerosol–radiation interactions. Phys Chem Minerals 39, 515–523 (2012). https://doi.org/10.1007/s00269-012-0507-y

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