CdSe Quantum-Dot-Sensitized Solar Cell with ∼100% Internal Quantum Efficiency

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Abstract
We have constructed and studied photoelectrochemical solar cells (PECs) consisting of a photoanode prepared by direct deposition of independently synthesized CdSe nanocrystal quantum dots (NQDs) onto a nanocrystalline TiO2 film (NQD/TiO2), aqueous Na2S or Li2S electrolyte, and a Pt counter electrode. We show that light harvesting efficiency (LHE) of the NQD/TiO2 photoanode is significantly enhanced when the NQD surface passivation is changed from tri-n-octylphosphine oxide (TOPO) to 4-butylamine (BA). In the PEC the use of NQDs with a shorter passivating ligand, BA, leads to a significant enhancement in both the electron injection efficiency at the NQD/TiO2 interface and charge collection efficiency at the NQD/electrolyte interface, with the latter attributed mostly to a more efficient diffusion of the electrolyte through the pores of the photoanode. We show that by utilizing BA-capped NQDs and aqueous Li2S as an electrolyte, it is possible to achieve ∼100% internal quantum efficiency of photon-to-electron conversion, matching the performance of dye-sensitized solar cells.