Foerster resonance energy transfer rate and local density of optical states are uncorrelated in any dielectric nanophotonic medium

TL;DR

This paper demonstrates that Foerster resonance energy transfer (FRET) rates are uncorrelated with the local density of optical states (LDOS) in dielectric nanophotonic media, challenging common assumptions and providing a new theoretical framework.

Contribution

The authors derive a theoretical model showing FRET rates are independent of LDOS and express FRET as a frequency integral of the Green function's imaginary part, applicable to arbitrary media.

Findings

FRET rate is constant at distances comparable to wavelength scale.

FRET is dominated by static dipole-dipole interaction, not LDOS.

Broadband LDOS has minimal impact on FRET rates.

Abstract

Motivated by the ongoing debate about nanophotonic control of Foerster resonance energy transfer (FRET), notably by the local density of optical states (LDOS), we study an analytic model system wherein a pair of ideal dipole emitters - donor and acceptor - exhibit energy transfer in the vicinity of an ideal mirror. The FRET rate is controlled by the mirror up to distances comparable to the donor-acceptor distance, that is, the few-nanometer range. For vanishing distance, we find a complete inhibition or a four-fold enhancement, depending on dipole orientation. For mirror distances on the wavelength scale, where the well-known `Drexhage' modification of the spontaneous-emission rate occurs, the FRET rate is constant. Hence there is no correlation between the Foerster (or total) energy transfer rate and the LDOS. At any distance to the mirror, the total energy transfer between a closely-spaced donor and acceptor is dominated by Foerster transfer, i.e., by the static dipole-dipole interaction that yields the characteristic inverse-sixth-power donor-acceptor distance dependence in homogeneous media. Generalizing to arbitrary inhomogeneous media with weak dispersion and weak absorption in the frequency overlap range of donor and acceptor, we derive two main theoretical results. Firstly, the spatially dependent Foerster energy transfer rate does not depend on frequency, hence not on the LDOS. Secondly the FRET rate is expressed as a frequency integral of the imaginary part of the Green function. This leads to an approximate FRET rate in terms of the LDOS integrated over a huge bandwidth from zero frequency to about 10 times the donor emission frequency, corresponding to the vacuum-ultraviolet. Even then, the broadband LDOS hardly contributes to the energy transfer rates. We discuss practical consequences including quantum information processing.