Excitation wavelength dependent photon anti-bunching/bunching from single quantum dots near gold nanostructures

Dey, Swayandipta; Zhou, Yadong; Sun, Yonglei; Jenkins, Julie A.; Kriz, David; Suib, Steven L.; Chen, Ou; Zou, Shengli; Zhao, Jing

doi:10.1039/C7NR05299E

Title: Excitation wavelength dependent photon anti-bunching/bunching from single quantum dots near gold nanostructures

Journal Article · Mon Jan 01 00:00:00 EST 2018 · Nanoscale

DOI:https://doi.org/10.1039/C7NR05299E· OSTI ID:1597851

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^[2]; Sun, Yonglei ^[1]; Jenkins, Julie A. ^[1]; Kriz, David ^[1];

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Univ. of Connecticut, Storrs, CT (United States)
Univ. of Central Florida, Orlando, FL (United States)
Brown Univ., Providence, RI (United States)

Here, we aim to investigate the change in photon emission statistics of single CdSe/CdS core/shell quantum dots (QDs) on dielectric modified gold nanoparticle (NP) substrates as a function of the excitation wavelength. Photons emitted from single QDs are typically “anti-bunched” and are independent of the excitation wavelength. However, when QDs are coupled to plasmonic substrates, even at the low excitation power regime, we observed a significant change in photoluminescence emission behavior of single QDs; i.e. the emission transformed from incomplete photon anti-bunched to bunched when the excitation was changed from “off” to “on” plasmon resonance. Theoretical studies based on electrodynamics modeling suggested that for the QD–Au NP system, the quantum yield of single excitons decreases while that of biexcitons increases. In addition, when excited at the “on” resonance condition, the absorption is highly enhanced, resulting in an increased population of higher order excitons of the QDs. The higher order exciton emission was directly observed as an additional peak appeared at the blue side of the exciton peak of single QDs. The combined effect of the change in quantum yield and the increase in the absorption cross-section switches the photons emitted by single QDs from anti-bunched to bunched. These results provided direct evidence that not only the plasmonic nanostructures but also the excitation wavelength can effectively control the photon emission statistics of single QDs in the hybrid metal–semiconductor system. Manipulating the multiexciton–plasmon interaction in a hybrid complex like this could possibly open up new doors for applications such as entangled photon pair generation and plasmon-enhanced optoelectronic devices.

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Research Organization:: Univ. of Connecticut, Storrs, CT (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)

Grant/Contract Number:: FG02-86ER13622; NSF CHE# 1554800

OSTI ID:: 1597851

Journal Information:: Nanoscale, Vol. 10, Issue 3; ISSN 2040-3364

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 12 works

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