Molecular-sized fluorescent nanodiamonds

Molecular-sized fluorescent nanodiamonds

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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


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Read our FAQs * Contact customer support SIMILAR CONTENT BEING VIEWED BY OTHERS SIMULTANEOUS LABEL-FREE LIVE IMAGING OF CELL NUCLEUS AND LUMINESCENT NANODIAMONDS Article Open access 17 June


2020 OPTICAL ACTIVATION AND DETECTION OF CHARGE TRANSPORT BETWEEN INDIVIDUAL COLOUR CENTRES IN DIAMOND Article 22 October 2021 SPATIALLY RESOLVED FLUORESCENCE OF CAESIUM LEAD HALIDE


PEROVSKITE SUPERCRYSTALS REVEALS QUASI-ATOMIC BEHAVIOR OF NANOCRYSTALS Article Open access 16 February 2022 REFERENCES * Mochalin, V. N., Shenderova, O., Ho, D. & Gogotsi, Y. The


properties and applications of nanodiamonds. _Nature Nanotech._ 7, 11–23 (2012). Article  CAS  Google Scholar  * Hui, Y. Y., Cheng, C-L. & Chang, H-C. Nanodiamonds for optical


bioimaging. _J. Phys._ 43, 374021 (2010). Google Scholar  * Barnard, A. S. & Sternberg, M. Substitutional nitrogen in nanodiamond and Bucky-diamond particles. _J. Phys. Chem. B_ 109,


17107–17112 (2005). Article  CAS  Google Scholar  * Wang, C., Kurtsiefer, C., Weinfurter, H. & Burchard, B. Single photon emission from SiV centres in diamond produced by ion


implantation. _J. Phys. B_ 39, 37–41 (2006). Article  Google Scholar  * Neu, E., Agio, M. & Becher, C. Photophysics of single silicon vacancy centers in diamond: implications for single


photon emission. _Opt. Express_ 20, 19956–19971 (2012). Article  CAS  Google Scholar  * Evanko, D. The new fluorescent probes on the block. _Nature Methods_ 5, 218–219 (2008). Article  CAS 


Google Scholar  * Biju, V., Itoh, T., Anas, A., Sujith, A. & Ishikawa, M. Semiconductor quantum dots and metal nanoparticles: syntheses, optical properties, and biological applications.


_Anal. Bioanal. Chem._ 391, 2469–2495 (2008). Article  CAS  Google Scholar  * Taylor, A., Wilson, K. M., Murray, P., Fernig, D. G. & Lévy, R. Long-term tracking of cells using inorganic


nanoparticles as contrast agents: are we there yet? _Chem. Soc. Rev._ 41, 2707–2717 (2012). Article  CAS  Google Scholar  * Barnard, A. S., Vlasov, I. I. & Ralchenko, V. G. Predicting


the distribution and stability of photoactive defect centers in nanodiamond biomarkers. _J. Mater. Chem._ 19, 360–365 (2009). Article  CAS  Google Scholar  * Raty, J-Y., Galli, G., Bostedt,


C., van Buuren, T. W. & Terminello, L. J. Quantum confinement and fullerenelike surface reconstructions in nanodiamonds. _Phys. Rev. Lett._ 90, 037401 (2003). Article  Google Scholar  *


Bolker, A., Saguy, C., Tordjman, M. & Kalish, R. Quantum confinement and Coulomb blockade in isolated nanodiamond crystallites. _Phys. Rev. B_ 88, 035442 (2013). Article  Google Scholar


  * Bradac, C. et al. Observation and control of blinking nitrogen-vacancy centres in discrete nanodiamonds. _Nature Nanotech._ 5, 345–349 (2010). Article  CAS  Google Scholar  * Vlasov, I.


I. et al. Nanodiamond photoemitters based on strong narrow-band luminescence from silicon-vacancy defects. _Adv. Mater._ 21, 808–812 (2009). Article  CAS  Google Scholar  * Lewis, R. S.,


Anders, E. & Draine, B. T. Properties, detectability and origin of interstellar diamonds in meteorites. _Nature_ 339, 117–121 (1989). Article  CAS  Google Scholar  * Daulton, T. L.,


Eisenhour, D. D., Bernatowicz, T. J., Lewis, R. S. & Buseck, P. R. Genesis of presolar diamonds: comparative high-resolution transmission electron microscopy study of meteoritic and


terrestrial nano-diamonds. _Geochim. Cosmochim. Acta_ 60, 4853–4872 (1996). Article  CAS  Google Scholar  * Shiryaev, A. A. et al. Spectroscopic study of impurities and associated defects in


nanodiamonds from Efremovka (CV3) and Orgueil (CI) meteorites. _Geochim. Cosmochim. Acta_ 75, 3155–3165 (2011). Article  CAS  Google Scholar  * Goss, J. P., Jones, R., Breuer, S. J.,


Briddon, P. R. & Öberg, S. The twelve-line 1.682 eV luminescence center in diamond and the vacancy-silicon complex. _Phys. Rev. Lett._ 77, 3041–3044 (1996). Article  CAS  Google Scholar


  * Erwin, S. C. et al. Doping semiconductor nanocrystals. _Nature_ 436, 91–94 (2005). Article  CAS  Google Scholar  * Chang, Y. K. et al. Quantum confinement effect in diamond nanocrystals


studied by X-ray-absorption spectroscopy. _Phys. Rev. Lett._ 82, 5377–5380 (1999). Article  CAS  Google Scholar  * Berg, T. et al. Quantum confinement observed in the X-ray absorption


spectrum of size distributed meteoritic nanodiamonds. _J. Appl. Phys._ 104, 064303 (2008). Article  Google Scholar  * Amari, S., Lewis, R. S. & Anders, E. Interstellar grains in


meteorites: I. Isolation of SiC, graphite and diamond; size distributions of SiC and graphite. _Geochim. Cosmochim. Acta_ 58, 459–470 (1994). Article  CAS  Google Scholar  * Clark, C. D.,


Kanda, H., Kiflawi, I. & Sittas, G. Silicon defects in diamond. _Phys. Rev. B_ 51, 16681–16688 (1995). Article  CAS  Google Scholar  * Neu, E. et al. Single photon emission from


silicon-vacancy colour centres in chemical vapour deposition nano-diamonds on iridium. _New J. Phys._ 13, 025012 (2011). Article  Google Scholar  * Sternschulte, H., Thonke, K., Sauer, R.,


Münzinger, P. & Michler, P. 1.681-eV luminescence center in chemical-vapor-deposited homoepitaxial diamond films. _Phys. Rev. B_ 50, 14554–14560 (1994). Article  CAS  Google Scholar  *


Krichevsky, O. & Bonnet, G. Fluorescence correlation spectroscopy: the technique and its applications. _Rep. Prog. Phys._ 65, 251–297 (2002). Article  CAS  Google Scholar  * Neugart, F.


et al. Dynamics of diamond nanoparticles in solution and cells. _Nano Lett._ 7, 3588–3591 (2007). Article  CAS  Google Scholar  * Kitson, S. C., Jonsson, P., Rarity, J. G. & Tapster, P.


R. Intensity fluctuation spectroscopy of small numbers of dye molecules in a microcavity. _Phys. Rev._ 58, 620–627 (1998). Article  CAS  Google Scholar  * Neu, E. et al. Narrowband


fluorescent nanodiamonds produced from chemical vapor deposition films. _Appl. Phys. Lett._ 98, 243107 (2011). Article  Google Scholar  * Gali, A. & Maze, J. R. An _ab initio_ study on


split silicon-vacancy defect in diamond: electronic structure and related properties. Preprint at http://arXiv.org/pdf/1310.2137 (2013). * Gali, A. Time-dependent density functional study on


the excitation spectrum of point defects in semiconductors. _Phys. Status Solidi B_ 248, 1337–1346 (2011). Article  CAS  Google Scholar  * Iakoubovskii, K., Adriaenssens, G. J., Dogadkin,


N. N. & Shiryaev, A. A. Optical characterization of some irradiation-induced centers in diamond. _Diam. Relat. Mater._ 10, 18–26 (2001). Article  CAS  Google Scholar  * Gendron, P-O.,


Avaltroni, F. & Wilkinson, K. J. Diffusion coefficients of several rhodamine derivatives as determined by pulsed field gradient–nuclear magnetic resonance and fluorescence correlation


spectroscopy. _J. Fluoresc._ 18, 1093–1101 (2008). Article  CAS  Google Scholar  * Müller, C. B. et al. Precise measurement of diffusion by multi-color dual-focus fluorescence correlation


spectroscopy. _EPL Eur. Lett._ 83, 46001 (2008). Article  Google Scholar  Download references 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. AUTHOR INFORMATION


AUTHORS AND AFFILIATIONS * General Physics Institute RAS, Vavilov Street 38, Moscow, 119991, Russia Igor I. Vlasov & Vitaly I. Konov * Institute of Physical Chemistry and


Electrochemistry RAS, Leninsky pr. 31, Moscow, 119071, Russia Andrey A. Shiryaev * 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 * Department of Atomic Physics, Budapest University of Technology and Economics, Budapest,


H-1111, Budafoki út 8, Hungary Márton Vörös & Adam Gali * Institute for Quantum Optics, University of Ulm, Albert-Einstein-Allee 11, Ulm, 89081, Germany Fedor Jelezko * Vernadsky


Institute of Geochemistry and Analytical Chemistry RAS, Kosygin Street 19, Moscow, Russia Anatolii V. Fisenko & Lubov F. Semjonova * Central Facility of Electron Microscopy, University


of Ulm, Albert-Einstein-Allee 11, Ulm, 89081, Germany Johannes Biskupek & Ute Kaiser * Laboratoire CRISMAT, UMR 6508 CNRS ENSICAEN, 6 boulevard Marechal Juin, Caen, 14050, France Oleg I.


Lebedev * Institute of Physics, University of Tartu, Riia Street 142, Tartu, 51014, Estonia Ilmo Sildos * Department of Electrical and Computer Engineering, 3128 Texas A&M University,


College Station, 77843-3128, Texas, USA Philip. R. Hemmer * 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 * Igor I. Vlasov View author publications You can also search for this author inPubMed Google Scholar * Andrey A. Shiryaev View author publications


You can also search for this author inPubMed Google Scholar * Torsten Rendler View author publications You can also search for this author inPubMed Google Scholar * Steffen Steinert View


author publications You can also search for this author inPubMed Google Scholar * Sang-Yun Lee View author publications You can also search for this author inPubMed Google Scholar * Denis


Antonov View author publications You can also search for this author inPubMed Google Scholar * Márton Vörös View author publications You can also search for this author inPubMed Google


Scholar * Fedor Jelezko View author publications You can also search for this author inPubMed Google Scholar * Anatolii V. Fisenko View author publications You can also search for this


author inPubMed Google Scholar * Lubov F. Semjonova View author publications You can also search for this author inPubMed Google Scholar * Johannes Biskupek View author publications You can


also search for this author inPubMed Google Scholar * Ute Kaiser View author publications You can also search for this author inPubMed Google Scholar * Oleg I. Lebedev View author


publications You can also search for this author inPubMed Google Scholar * Ilmo Sildos View author publications You can also search for this author inPubMed Google Scholar * Philip. R.


Hemmer View author publications You can also search for this author inPubMed Google Scholar * Vitaly I. Konov View author publications You can also search for this author inPubMed Google


Scholar * Adam Gali View author publications You can also search for this author inPubMed Google Scholar * Jörg Wrachtrup View author publications You can also search for this author


inPubMed Google Scholar 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. CORRESPONDING AUTHOR Correspondence to Jörg Wrachtrup. ETHICS DECLARATIONS


COMPETING INTERESTS The authors declare no competing financial interests. SUPPLEMENTARY INFORMATION SUPPLEMENTARY INFORMATION Supplementary Information (PDF 1376 kb) RIGHTS AND PERMISSIONS


Reprints and permissions ABOUT THIS ARTICLE CITE THIS ARTICLE 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 Download citation * Received: 24 June 2013 * Accepted: 28 October 2013 * Published: 08 December 2013 * Issue Date: January 2014 * DOI:


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