Body-of-revolution finite-element model of plasmon-enhanced fluorescence

Abstract

Plasmon-enhanced fluorescence (PEF) is one of the most widely investigated optical phenomena in hybrid systems of emitters and plasmonic nanoantennas, with applications ranging from biosensing to single-molecule emission microscopy. However, the computational optimisation of these systems is frequently hindered by the substantial memory and computational costs associated with full three-dimensional (3D) electromagnetic simulations. In this work, we extend finite-element modelling of PEF beyond spherically symmetric geometries using a body-of-revolution finite-element method (BOR-FEM). By exploiting exact or equivalent rotational symmetry, 3D emitter–nanoantenna systems are reduced to computationally efficient 2D formulations while retaining the essential electromagnetic interactions governing excitation and emission. We validate the framework against three previously investigated emitter–nanorod systems, including one requiring an equivalent axisymmetric geometric transformation, before applying it to an emitter–core–shell nanorod system. Specifically, we investigate the PEF of the terminal chlorophyll emitter of the major plant light-harvesting complex (LHCII), the most abundant membrane protein on Earth, interacting with a gold core-dielectric shell nanorod with one or two dielectric shells. The simulations reveal that the interplay between excitation enhancement, radiativerate enhancement, and non-radiative Ohmic losses gives rise to four distinct shell-thickness-dependent operating regimes (quenching, enhancement, suppression, and decoupling), with recovery of the intrinsic quantum yield in the decoupling regime. The predicted enhancement factors for experimentally relevant dual-shell nanorods agree well with previously reported measurements. These results establish BOR-FEM as an efficient and versatile framework for modelling PEF in rotationally-symmetric nanoantenna geometries and in non-axisymmetric geometries that admit equivalent axisymmetric representations, providing a practical route for the rational design and optimisation of plasmon-enhanced bio-nanophotonic systems.