Singlet fission photovoltaics

Abstract

The efficiency of a solar cell is restricted by the "single junction limit," whereby photons with energy higher than the bandgap lose energy by thermalization. Singlet exciton fission splits a high-energy molecular excitation ("singlet" exciton) into a pair of lowenergy ones ("triplet" excitons). In solar cells, it promises to generate two electrons per photon, potentially overcoming the singlet junction efficiency limit. In this thesis, we present singlet-fission-based photovoltaic cells that generate more than one electron per photon. We first demonstrate organic photodetectors with quantum efficiencies reaching 100% by exploiting singlet exciton fission. Through study of the magnetic field dependence of the fission process, we find an optimum thickness of singlet fission layers that guarantees the nearly 100% conversion of a singlet into two triplets. By employing an exciton blocking layer and a light trapping scheme to the solar cell, we demonstrate the peak external quantum efficiency exceeding 100% in the visible spectrum. It is the first time that any solar cell has generated more than one electron per photon outside the UV spectrum. We also build a simple model that predicts the rate of singlet fission through intermolecular coupling, enabling rational designs of singlet fission molecules and devices. Finally, we propose a future direction-generating three electrons per photon. As a step toward this goal, we demonstrate singlet exciton fission in hexacene, whose energetics may allow a singlet to split into three triplets.