Dielectric polarization, anisotropy and nonradiative energy transfer into nanometre-scale thin semiconducting films

Abstract

A common problem of nonradiative energy transfer (NRET) from a small energy donor into a neighbouring energy acceptor layer is addressed with the emphasis on the layer thickness dependence. Two complementary approaches are employed to study dielectric polarization effects on NRET into thin films: a macroscopic analysis treating the acceptor layer as a continuum characterized by a frequency-dependent dielectric function, and a direct modelling utilizing discrete acceptor lattices, each of the acceptors being a polarizable point dipole. Explicit illustrations are provided of an interesting phenomenon, when NRET into thinner films can counter-intuitively be more efficient than NRET into thicker films. We show that this phenomenon may take place for a broad range of the acceptor polarization responses, including metallic-like and insulating behaviour as well as responses with weak and strong dissipation. The spectral vicinity of a strong dielectric resonance in the acceptor layer is studied as a specific example. The role of geometry-derived and intrinsic anisotropy of the acceptor response is clarified in the illustrations. Our results suggest that NRET optimization might be possible in the design of hybrid nanostructures, where the geometry of the structures is better matched with spectral properties of donor and acceptor subsystems.