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Localized surface plasmon resonances arising from free carriers in doped quantum dots

Nature Materials volume 10, pages 361–366 (2011)Cite this article

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Abstract

Localized surface plasmon resonances (LSPRs) typically arise in nanostructures of noble metals1,2 resulting in enhanced and geometrically tunable absorption and scattering resonances. LSPRs, however, are not limited to nanostructures of metals and can also be achieved in semiconductor nanocrystals with appreciable free carrier concentrations. Here, we describe well-defined LSPRs arising from p-type carriers in vacancy-doped semiconductor quantum dots (QDs). Achievement of LSPRs by free carrier doping of a semiconductor nanocrystal would allow active on-chip control of LSPR responses. Plasmonic sensing and manipulation of solid-state processes in single nanocrystals constitutes another interesting possibility. We also demonstrate that doped semiconductor QDs allow realization of LSPRs and quantum-confined excitons within the same nanostructure, opening up the possibility of strong coupling of photonic and electronic modes, with implications for light harvesting, nonlinear optics, and quantum information processing.

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Figure 1: Localized surface plasmon resonance (LSPR) frequency dependence on free carrier density and doping constraints.
Figure 2: Size-controlled synthesis of copper(I) sulphide QDs.
Figure 3: Excitons and localized surface plasmon resonances in absorbance spectra of Cu2−xS quantum dots.
Figure 4: Active tuning of LSPRs in Cu(I)S nanorods by introduction of copper vacancies.

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Acknowledgements

Work on copper sulphide nanocrystal synthesis and optical and structural characterization was supported by the Physical Chemistry of Semiconductor Nanocrystals Program, KC3105, Director, Office of Science, Office of Basic Energy Sciences, of the United States Department of Energy under contract DE-AC02-05CH11231. Work on LSPR response characterization, chemical tuning, and vacancy density profiling was supported by a Miller Fellowship awarded to P.K.J. We thank J. Owen, J. B. Rivest and J. van de Lagemaat for discussions and Lam-Kiu Fong for a CdS nanorod sample.

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Author notes

  1. Joseph M. Luther and Prashant K. Jain: These authors contributed equally to this work

Authors and Affiliations

  1. Department of Chemistry, University of California, Berkeley, California 94720, USA

    Joseph M. Luther, Prashant K. Jain, Trevor Ewers & A. Paul Alivisatos

  2. Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 947203, USA

    Joseph M. Luther, Prashant K. Jain, Trevor Ewers & A. Paul Alivisatos

  3. Miller Institute for Basic Research in Science, University of California, Berkeley, California 94720, USA

    Prashant K. Jain

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  1. Joseph M. Luther
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Contributions

J.M.L. and P.K.J. contributed equally to this work. J.M.L. synthesized copper sulphide quantum dots and performed optical characterization. P.K.J. performed work on LSPR characterization and assignment; Cu(I)S crystallography and vacancy profiling; and active chemical tuning of LSPRs. T.E. performed electron microscopy of copper sulphide nanocrystals. J.M.L., P.K.J., T.E., and A.P.A. discussed results and prepared the manuscript and subsequent revisions.

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Correspondence to A. Paul Alivisatos.

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Luther, J., Jain, P., Ewers, T. et al. Localized surface plasmon resonances arising from free carriers in doped quantum dots. Nature Mater 10, 361–366 (2011). https://doi.org/10.1038/nmat3004

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