Picosecond Lifetimes with High Quantum Yields from Single-Photon-Emitting Colloidal Nanostructures at Room Temperature.

Abstract

Minimizing the luminescence lifetime while maintaining a high emission quantum yield is paramount in optimizing the excitation cross-section, radiative decay rate, and brightness of quantum solid-state light sources, particularly at room temperature, where nonradiative processes can dominate. We demonstrate here that DNA-templated 60 and 80 nm diameter gold nanoparticle dimers, featuring one fluorescent molecule, provide single-photon emission with lifetimes that can fall below 10 ps and typical quantum yields in a 45-70% range. Since these colloidal nanostructures are obtained as a purified aqueous suspension, fluorescence spectroscopy can be performed on both fixed and freely diffusing nanostructures to quantitatively estimate the distributions of decay rate and fluorescence intensity enhancements. These data are in excellent agreement with theoretical calculations and demonstrate that millions of bright fluorescent nanostructures, with radiative lifetimes below 100 ps, can be produced in parallel.