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Molecular-sized fluorescent nanodiamonds

Nature Nanotechnology volume 9, pages 54–58 (2014)Cite this article

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Abstract

Doping of carbon nanoparticles with impurity atoms is central to their application1,2. However, doping has proven elusive for very small carbon nanoparticles because of their limited availability and a lack of fundamental understanding of impurity stability in such nanostructures3. Here, we show that isolated diamond nanoparticles as small as 1.6 nm, comprising only ∼400 carbon atoms, are capable of housing stable photoluminescent colour centres, namely the silicon vacancy (SiV)4,5. Surprisingly, fluorescence from SiVs is stable over time, and few or only single colour centres are found per nanocrystal. We also observe size-dependent SiV emission supported by quantum-chemical simulation of SiV energy levels in small nanodiamonds. Our work opens the way to investigating the physics and chemistry of molecular-sized cubic carbon clusters and promises the application of ultrasmall non-perturbative fluorescent nanoparticles as markers in microscopy and sensing.

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Figure 1: Structure of SiV centre in diamond.
Figure 2: Photoluminescence analysis of the meteoric nanodiamonds.
Figure 3: HRTEM analysis of meteoritic nanodiamonds.
Figure 4: FCS measurement of luminescent meteoritic nanodiamonds and a dye molecule (Rhodamine 6G (Rh 6G)).
Figure 5: Detailed analysis of a fluorescent spot presumably containing only few emitters.

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Acknowledgements

This work was supported in part by Russian Foundation for Basic Research (RFBR) grants nos 11-02-01432, 12-05-00208 and 12-03-00787, a grant from Russian Academy of Science (RAS) programme no. 24, a grant of the President of the Russian Federation for leading scientific schools (no. 3076.2012.2), an National Institutes of Health (NIH) grant (no. C09-00053), the European Commission, EU FP7 grants Diamond based atomic nanotechnologies (DIAMANT) and Development of diamond intracellular nanoprobes for oncogen transformation dynamics monitoring in living cells (DINAMO), as well as the European Research Council (ERC) (via project Spin Quantum Technologies (SQUTEC) Biology and Quantum (BioQ)), the Deutsche Forschungsgemeinschaft (DFG) (via Sonderforschungsbereiches (SFB) 716) and the Volkswagenstiftung.

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Authors and Affiliations

  1. General Physics Institute RAS, Vavilov Street 38, Moscow, 119991, Russia

    Igor I. Vlasov & Vitaly I. Konov

  2. Institute of Physical Chemistry and Electrochemistry RAS, Leninsky pr. 31, Moscow, 119071, Russia

    Andrey A. Shiryaev

  3. 3rd Physical Institute and Research Center SCOPE, University of Stuttgart, Pfaffenwaldring 57, Stuttgart, 70550, Germany

    Torsten Rendler, Steffen Steinert, Sang-Yun Lee, Denis Antonov & Jörg Wrachtrup

  4. Department of Atomic Physics, Budapest University of Technology and Economics, Budapest, H-1111, Budafoki út 8, Hungary

    Márton Vörös & Adam Gali

  5. Institute for Quantum Optics, University of Ulm, Albert-Einstein-Allee 11, Ulm, 89081, Germany

    Fedor Jelezko

  6. Vernadsky Institute of Geochemistry and Analytical Chemistry RAS, Kosygin Street 19, Moscow, Russia

    Anatolii V. Fisenko & Lubov F. Semjonova

  7. Central Facility of Electron Microscopy, University of Ulm, Albert-Einstein-Allee 11, Ulm, 89081, Germany

    Johannes Biskupek & Ute Kaiser

  8. Laboratoire CRISMAT, UMR 6508 CNRS ENSICAEN, 6 boulevard Marechal Juin, Caen, 14050, France

    Oleg I. Lebedev

  9. Institute of Physics, University of Tartu, Riia Street 142, Tartu, 51014, Estonia

    Ilmo Sildos

  10. Department of Electrical and Computer Engineering, 3128 Texas A&M University, College Station, 77843-3128, Texas, USA

    Philip. R. Hemmer

  11. Institute for Solid State Physics and Optics, Wigner Research Centre for Physics, Hungarian Academy of Sciences, PO Box 49, Budapest, 1525, Hungary

    Adam Gali

Authors
  1. Igor I. Vlasov
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Contributions

I.V., J.W., P.H. and F.J. designed and coordinated the experiment. I.V., A.A.S., L.F.S., A.V.F., O.I.L., V.I.K. and I.S. prepared and characterized the sample. U.K. and J.B. carried out the high-resolution electron microscopy. T.R., S.S. and S.Y.L. designed, set up and carried out fluorescence measurements. A.G., D.A. and M.V. carried out the calculations and analysed the simulation data. I.V., T.R., S.Y.L., A.G., P.H. and J.W. wrote the manuscript.

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Correspondence to Jörg Wrachtrup.

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Vlasov, I., Shiryaev, A., Rendler, T. et al. Molecular-sized fluorescent nanodiamonds. Nature Nanotech 9, 54–58 (2014). https://doi.org/10.1038/nnano.2013.255

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