Bawendi, Quantization of Multiparticle Auger Rates in Semiconductor Quantum Dots, Science., 2000, 287, 1011–1013. Klimov, Mechanisms for Photogeneration and Recombination of Multiexcitons in Semiconductor Nanocrystals: Implications for Lasing and Solar Energy Conversion, J. Klimov, High Efficiency Carrier Multiplication in PbSe Nanocrystals: Implications for Solar Energy Conversion, Phys. 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. 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/SiO 2. The probability of single-photon emission of single QD was increased by the enhancement of the excitation rate via adjusting the distance using Ag/SiO 2 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 fabricating well-defined SiO 2-coated AgNPs and AuNPs (metal/SiO 2), the spectral overlap originated from the metal species of Ag and Au and the distance constituted by the thickness of the SiO 2 shell are controlled. 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. 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. Emission photon statistics, i.e., single-photon and multi-photon emissions, of isolated QDs is required for tailoring optoelectronic applications.
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