Solid-state infrared-to-visible upconversion for sub-bandgap sensitization of photovoltaics

By harvesting sub-bandgap photons, we have a path to overcome the Shockley-Queisser limit in photovoltaics (PVs). We investigate semiconductor nanocrystal (NC) sensitized upconversion via triplet-triplet annihilation (TTA) in organic semiconductors (OSCs). Since this process relies on optically inactive triplet states in the OSCs, we utilize PbS NCs to directly sensitize the triplet state via energy transfer. This is possible due to the strong spin-orbit coupling in PbS NCs, resulting in rapid spin-dephasing of the exciton. Current technology allows for upconversion of light with a photon energy above $\sim 1.1$ eV. However, while internal efficiencies are rapidly improving, the low external device efficiencies render them impractical for applications, as devices are based on a single monolayer of NCs. Our results show simply increasing the PbS NC film thickness does not show improvement in the efficiency due to poor exciton transport between PbS NCs. Here, we present a new strategy to increase the external upconversion efficiency by utilizing thin tinbased halide perovskites as the absorbing layer. Resonant energy transfer from the perovskite to the PbS NCs allows for subsequent sensitization of the triplet state in rubrene.