Synergy of Excitation Enhancement and the Purcell Effect for Strong Photoluminescence Enhancement in a Thin-Film Hybrid Structure Based on Quantum Dots and Plasmon Nanoparticles

J Phys Chem Lett. 2020 Oct 1;11(19):8018-8025. doi: 10.1021/acs.jpclett.0c02296. Epub 2020 Sep 11.

Abstract

Reliable control of spontaneous radiation from quantum emitters, such as quantum dots (QDs), is an extremely important problem in quantum science, nanophotonics, and engineering. The QD photoluminescence (PL) may be enhanced near plasmon nanoparticles because of excitation field enhancement or the Purcell effect. However, both of these effects have their specific limitations. The excitation enhancement is usually accompanied by a decrease in the PL quantum yield (QY) due to the plasmon-induced energy transfer, and the Purcell effect cannot significantly enhance the PL of QDs with an initially high QY because of the obvious limitation of the QY by the value of 100%. Here, we have shown that the synergistic combination of excitation enhancement caused by silver nanospheres and the Purcell effect caused by silver nanoplates in the same QD-in-polymer hybrid thin-film nanostructure permits simultaneous increases in the radiative and excitation rates to be obtained. This overcomes the limitations of each individual effect and yields a synergistic PL increase (+1320%) greater than the sum of the PL enhancements determined by each effect alone (+70% and +360%).