Title: Improved Energy Pooling Efficiency Through Inhibited Spontaneous Emission,
Abstract: The radiative lifetime of molecules or atoms can be increased by placing them
within a tuned conductive cavity that inhibits spontaneous emission. This was
examined as a possible means of enhancing three-body, singlet-based
upconversion, known as energy pooling. Achieving efficient upconversion of
light has potential applications in the fields of photovoltaics, biofuels, and
medicine. The affect of the photonically constrained environment on pooling
efficiency was quantified using a kinetic model populated with data from
molecular quantum electrodynamics, perturbation theory, and ab initio
calculations. This model was applied to a system with fluorescein donors and a
hexabenzocoronene acceptor. Placing the molecules within a conducting cavity
was found to increase the efficiency of energy pooling by increasing both the
donor lifetime and the acceptor emission rate--i.e. a combination of inhibited
spontaneous emission and the Purcell effect. A model system with a free-space
pooling efficiency of 23% was found to have an efficiency of 47% in a
rectangular cavity.