Abstract

Typical emitters such as molecules, quantum dots and semiconductor quantum wells have slow spontaneous emission with lifetimes of 1–10 ns, creating a mismatch with high-speed nanoscale optoelectronic devices such as light-emitting diodes, single-photon sources and lasers. Here we experimentally demonstrate an ultrafast (<11 ps) yet efficient source of spontaneous emission, corresponding to an emission rate exceeding 90 GHz, using a hybrid structure of single plasmonic nanopatch antennas coupled to colloidal quantum dots. The antennas consist of silver nanocubes coupled to a gold film separated by a thin polymer spacer layer and colloidal core–shell quantum dots, a stable and technologically relevant emitter. We show an increase in the spontaneous emission rate of a factor of 880 and simultaneously a 2,300-fold enhancement in the total fluorescence intensity, which indicates a high radiative quantum efficiency of ∼50%. The nanopatch antenna geometry can be tuned from the visible to the near infrared, providing a promising approach for nanophotonics based on ultrafast spontaneous emission.

Highlights

  • Typical emitters such as molecules, quantum dots and semiconductor quantum wells have slow spontaneous emission with lifetimes of 1–10 ns, creating a mismatch with high-speed nanoscale optoelectronic devices such as light-emitting diodes, single-photon sources and lasers

  • The nanopatch antennas (NPAs) system consists of a silver nanocube coupled to a metal film, separated by a controlled nanoscale (B10 nm) dielectric spacer layer and colloidal quantum dots (QDs) (Fig. 1a–c)

  • The fundamental plasmonic mode is a Fabry–Perot resonance resulting from multiple reflections of the waveguide mode beneath the nanocube that propagates within the gap region

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Summary

Introduction

Typical emitters such as molecules, quantum dots and semiconductor quantum wells have slow spontaneous emission with lifetimes of 1–10 ns, creating a mismatch with high-speed nanoscale optoelectronic devices such as light-emitting diodes, single-photon sources and lasers. We experimentally demonstrate an ultrafast (o11 ps) yet efficient source of spontaneous emission, corresponding to an emission rate exceeding 90 GHz, using a hybrid structure of single plasmonic nanopatch antennas coupled to colloidal quantum dots. We show an increase in the spontaneous emission rate of a factor of 880 and simultaneously a 2,300-fold enhancement in the total fluorescence intensity, which indicates a high radiative quantum efficiency of B50%. Colloidal QDs have been demonstrated as stable, room temperature singlephoton sources[2,3], but the slow radiative rate associated with these systems limits the attainable repetition rate.

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