Realistic Efficiency Limits for Singlet-Fission Silicon Solar Cells

Singlet fission is a carrier multiplication mechanism that could make silicon solar cells much more efficient. The singlet-fission process splits one high-energy spin-singlet exciton into two lower-energy spin-triplet excitons. We calculated the efficiency potential of three technologically relevant singlet-fission silicon solar cell implementations. We assume realistic but optimistic parameters for the singlet-fission material and investigate the effect of singlet energy and entropic gain. If the transfer of triplet excitons occurs via charge transfer, the maximum efficiency is 34.6% at a surprisingly small singlet energy of 1.85 eV. For the Dexter-type triplet energy transfer, the maximum efficiency is 32.9% at a singlet energy of 2.15 eV. For Förster resonance energy transfer (FRET), the triplet excitons are first transferred into a quantum dot, from which they then undergo FRET into silicon. For this transfer mechanism, the maximum efficiency is 28.% at a singlet energy of 2.33 eV. We show that the efficiency gain from singlet fission is larger the more efficient the silicon base cell is, which stands in contrast to tandem perovskite-silicon solar cells.