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Modification of emission photon statistics from single quantum dots using metal/SiO2 core/shell nanostructures

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Abstract

Emission photon statistics, i.e., single-photon and multi-photon emissions, of isolated QDs is required for tailoring optoelectronic applications. In this article, we demonstrate that the emission photon statistics can be modified by the control of the spectral overlap of the QDs with the localized surface plasmon resonance (LSPR) of the metal nanoparticle (metal NP) and by the distance between the QD and the metal NP. Moreover, the contribution to the modification of the emission photon statistics, which is the excitation and emission enhancements and the quenching generated by the spectral overlap and the distance, is elucidated. By fabricating well-defined SiO2-coated AgNPs and AuNPs (metal/SiO2), the spectral overlap originated from the metal species of Ag and Au and the distance constituted by the thickness of the SiO2 shell are controlled. The probability of single-photon emission of single QD was increased by the enhancement of the excitation rate via adjusting the distance using Ag/SiO2 while the single-photon emission was converted to multi-photon emission by the effect of exciton quenching at a short distance and a small spectral overlap. By contrast, the probability of multi-photon emission was increased by enhancement of the multi-photon emission rate and the quenching via the spectral overlap using Au/SiO2. These results indicated the fundamental finding to control emission photon statistics in single QDs by controlling the spectral overlap and the distance, and understand the interaction of plasmonic nanostructures and single QD systems.

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Acknowledgments

This work was partly supported by a Grant-in-Aid for Scientific Research on Priority Area “Strong Photons-Molecules Coupling Fields (No. 470)”; from the Ministry of Education, Culture, Sports, Science and Technology, Japan, a Grant-in-Aid for the Japan Society for the Promotion of Science (JSPS) Fellows (No. 12J08034 to HN) and a Grant-in-Aid for Scientific Research (No. 26390023 to SM) from JSPS. Additionally, we wish to thank Professor Dr Hitoshi Kasai and Assistant Professor Dr Tsunenobu Onodera at Tohoku University for preparation and characterization of metal/SiO2-QD systems and Professor Dr Noriaki Ikeda at the Kyoto Institute of Technology for use of their measurement setup.

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Authors and Affiliations

  1. Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Katahira 2-1-1, Aoba-ku, Sendai, 980-8577, Japan

    Hiroyuki Naiki & Hidetoshi Oikawa

  2. Department of Applied Chemistry for Environment, Kwansei Gakuin University, Gakuen 2-1, Sanda, Hyogo, 669-1337, Japan

    Sadahiro Masuo

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  1. Hiroyuki Naiki
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Naiki, H., Oikawa, H. & Masuo, S. Modification of emission photon statistics from single quantum dots using metal/SiO2 core/shell nanostructures. Photochem Photobiol Sci 16, 489–498 (2017). https://doi.org/10.1039/c6pp00342g

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