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Magnetic polaron on dangling-bond spins in CdSe colloidal nanocrystals

Nature Nanotechnology volume 12, pages 569–574 (2017)Cite this article

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Abstract

Non-magnetic colloidal nanostructures can demonstrate magnetic properties typical for diluted magnetic semiconductors because the spins of dangling bonds at their surface can act as the localized spins of magnetic ions. Here we report the observation of dangling-bond magnetic polarons (DBMPs) in 2.8-nm diameter CdSe colloidal nanocrystals (NCs). The DBMP binding energy of 7 meV is measured from the spectral shift of the emission lines under selective laser excitation. The polaron formation at low temperatures occurs by optical orientation of the dangling-bond spins (DBSs) that result from dangling-bond-assisted radiative recombination of spin-forbidden dark excitons. Modelling of the temperature dependence of the DBMP-binding energy and emission intensity shows that the DBMP is composed of a dark exciton and about 60 DBSs. The exchange integral of one DBS with the electron confined in the NC is ∼0.12 meV.

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Figure 1: FLN.
Figure 2: Polaron formation.
Figure 3: Dynamics under long-term illumination.
Figure 4: Temperature dependences: experiment and theory.

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Change history

  • 23 March 2017

    In the version of this Article originally published, in Fig. 3b the uppermost y axis tick mark label should have read '8.5' This has been corrected in all versions of the Article.

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Acknowledgements

A.L.E. acknowledges financial support of the Office of Naval Research through the Naval Research Laboratory Basic Research Program and Alexander-von-Humboldt Foundation. E.V.S., A.V.R., D.R.Y. and M.B. acknowledge support from the Deutsche Forschungsgemeinschaft via Sonderforschungsbereich TRR 160 and of the Government of Russia (project number 14.Z50.31.0021, leading scientist M. Bayer). Z.H. and B.D. acknowledge support by the European Commission via the Marie-Sklodowska Curie action Phonsi (H2020-MSCA-ITN-642656). Z.H. acknowledges support by the Belgian Science Policy Office (IAP 7.35, photonics@be) and Ghent University (GOA n01G01513). We thank M. M. Glazov for stimulating discussions.

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Authors and Affiliations

  1. Experimentelle Physik 2, Technische Universität Dortmund, Dortmund, 44227, Germany

    Louis Biadala, Elena V. Shornikova, Dmitri R. Yakovlev, Benjamin Siebers & Manfred Bayer

  2. IEMN, CNRS, Avenue Henri Poincaré, Villeneuve-d'Ascq, 59491, France

    Louis Biadala

  3. Rzhanov Institute of Semiconductor Physics, Siberian Branch of Russian Academy of Sciences, Novosibirsk, 630090, Russia

    Elena V. Shornikova

  4. Ioffe Institute, Russian Academy of Sciences, Saint Petersburg, 194021, Russia

    Anna V. Rodina, Dmitri R. Yakovlev & Manfred Bayer

  5. Department of Inorganic and Physical Chemistry, Universiteit Gent, Ghent, 9000, Belgium

    Tangi Aubert & Zeger Hens

  6. Laboratoire de Physique et d'Etude des Matériaux, PSL Research University, CNRS UMR 8213, Sorbonne Universités UPMC Université Paris 06, ESPCI Paris, 10 rue Vauquelin, Paris, 75005, France

    Michel Nasilowski & Benoit Dubertret

  7. Naval Research Laboratory, Washington, 20375, DC, USA

    Alexander L. Efros

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Contributions

L.B., E.V.S. and B.S. performed the measurements under the guidance of D.R.Y. and M.B. A.V.R. and A.L.E. developed the theoretical model. L.B., E.V.S., A.V.R., D.R.Y. and A.L.E. analysed and interpreted the data. T.A. and M.N. synthesized the NCs under the guidance of Z.H. and B.D. L.B., E.V.S., A.V.R., D.R.Y. and A.L.E. wrote the manuscript with the assistance of all other co-authors.

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Correspondence to Louis Biadala, Anna V. Rodina or Dmitri R. Yakovlev.

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The authors declare no competing financial interests.

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Biadala, L., Shornikova, E., Rodina, A. et al. Magnetic polaron on dangling-bond spins in CdSe colloidal nanocrystals. Nature Nanotech 12, 569–574 (2017). https://doi.org/10.1038/nnano.2017.22

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