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Radio-colouration of diamond: a spectroscopic study

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Abstract

We have undertaken a study of the common green or orange-brown spots at the surface of rough diamond specimens, which are caused by alpha particles emanating from radioactive sources outside the diamond. Richly coloured haloes represent elevated levels of structural damage, indicated by strong broadening of the main Raman band of diamond, intense strain birefringence, and up-doming of spots due to their extensive volume expansion. Green radio-colouration was analogously generated through the irradiation of diamond with 8.8 MeV helium ions. The generation of readily visible radio-colouration was observed after irradiating diamond with ≥1015 He ions per cm2. The accumulation of such a high number of alpha particles requires irradiation of the diamond from a radioactive source over long periods of time, presumably hundreds of millions of years in many cases. In the samples irradiated with He ions, amorphisation was observed in volume areas where the defect density exceeded 5 × 10−3 Å−3 (or 0.03 dpa; displacements per target atom). In contrast, graphitisation as a direct result of the ion irradiation was not observed. The green colouration transformed to brown at moderate annealing temperatures (here 450 °C). The colour transformation is associated with only partial recovery of the radiation damage. The colour change is mainly due to the destruction of the GR1 centre, explained by trapping of vacancies at A defects to form the H3 centre. An activation energy of ~2.4 ± 0.2 eV was determined for the GR1 reduction. The H3 centre, in turn, causes intense yellowish-green photoluminescence under ultraviolet illumination. Radio-colouration and associated H3 photoluminescence are due to point defects created by the ions irradiated, whereas lattice ionisation is of minor importance. This is concluded from the depth distribution of the colouration and the photoluminescence intensity (which corresponds to the defect density but not the ionisation distribution pattern). The effect of the implanted He ions themselves on the colour and photoluminescence seems to be negligible, as radio-colouration and H3 emission were analogously produced through irradiation of diamond with C ions. The photoluminescence emission becomes observable at extremely low defect densities on the order of 10−6 Å−3 (or 0.000006 dpa) and is suppressed at moderate defect densities of ~5 × 10−4 Å−3 (or ~0.003 dpa). Intensely brown-coloured diamond hence does not show the H3 emission anymore. Anneals up to 1,600 °C has reduced considerably irradiation damage and radio-colouration, but the structural reconstitution of the diamond (and its de-colouration) was still incomplete.

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Acknowledgments

DeBeers Consolidated Mines Ltd. is thanked for making available diamond specimens for irradiation experiments. Diamond crystals from Thailand were kindly provided by Somruedee Satitkune. We are grateful to Andreas Wagner and Wolfgang Zirbs for technical assistance and to Robert Stark for providing access to his laboratory for AFM measurements. Rainer Grötzschel, Viton Heera, Adrian Jones, John I. Koivula, Matthias Posselt, and Heinz Surbeck are thanked for stimulating discussions. Constructive reviews of two anonymous experts are gratefully acknowledged. This research was supported financially by the European Commission through contract no. MEXC–CT–2005–024878 and Research Infrastructures Transnational Access (RITA) grant no. 025646, and the Austrian Science Fund (FWF) through grants P20028–N10 and P24448–N19, to L.N.

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Authors and Affiliations

  1. Institut für Mineralogie und Kristallographie, Universität Wien, Althanstr. 14, 1090, Wien, Austria

    Lutz Nasdala & Manfred Wildner

  2. Institut für Ionenstrahlphysik und Materialforschung, Forschungszentrum Dresden-Rossendorf e.V., P.O. Box 510119, 01314, Dresden, Germany

    Dieter Grambole

  3. Sektion Kristallographie, Ludwig-Maximilians-Universität München, 80333, Munich, Germany

    Alexander M. Gigler

  4. Gemlab Gemological Laboratory, 9496, Balzers, Liechtenstein

    Thomas Hainschwang

  5. Department of Engineering Science and Physics, College of Staten Island, Staten Island, NY, 10314, USA

    Alexander M. Zaitsev

  6. School of Geographical and Earth Sciences, University of Glasgow, Glasgow, G12 8QQ, UK

    Jeffrey W. Harris

  7. Department of Earth Sciences, University College London, London, WC1E 6BT, UK

    Judith Milledge

  8. Department of Geology, University of Toronto Mississauga, Toronto, ON, M5S 3B1, Canada

    Daniel J. Schulze

  9. Institut für Geowissenschaften, Johannes Gutenberg-Universität Mainz, 55099, Mainz, Germany

    Wolfgang Hofmeister

  10. Department of Geology, Faculty of Science, Chulalongkorn University, Bangkok, 10330, Thailand

    Walter A. Balmer

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  1. Lutz Nasdala
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Correspondence to Lutz Nasdala.

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Communicated by J. Hoefs.

This article is dedicated to George Bosshart (1943–2012), who since the late 1980s had devoted most of his research activities to the study of processes causing natural and artificial green diamond colouration. His contributions to diamond research have stimulated also the investigation presented here.

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Nasdala, L., Grambole, D., Wildner, M. et al. Radio-colouration of diamond: a spectroscopic study. Contrib Mineral Petrol 165, 843–861 (2013). https://doi.org/10.1007/s00410-012-0838-1

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