Simultaneously giant enhancement of Forster resonance energy transfer rate and efficiency based on plasmonic excitations

TL;DR

This paper demonstrates that plasmonic excitations in nanoparticle clusters can dramatically enhance FRET rate and efficiency, revealing new insights into their dependence on local optical properties.

Contribution

It provides first-principles calculations showing simultaneous giant enhancement of FRET rate and efficiency using plasmonic hotspots, clarifying the LDOS dependence.

Findings

FRET rate can be enhanced by over 9 orders of magnitude.

FRET efficiency can be increased by over 3 orders of magnitude.

The study reveals conditions where FRET rate is independent or dependent on LDOS.

Abstract

We present a first-principles calculation on the rate and efficiency of F\"orster resonance energy transfer (FRET) from a donor to an acceptor when they are located in the hotspots of nanoparticle clusters. Nonlocal effect has been considered by using a hydrodynamic model. It is found that FRET rate and efficiency can be enhanced simultaneously by more than 9 and 3 orders of magnitude, respectively. The physical origins for these phenomena have been disclosed. Two opposite phenomena, the energy transfer rate is independent or dependent of the local density of optical states (LDOS), have been observed in the same system under different conditions. These findings not only help us to understand the unresolved debate on how the FRET rate depends on the LDOS, but also provide a new way to realize ultrafast energy transfer process with ultrahigh efficiency.