Suppressed Interfacial Charge Recombination of PbS Quantum Dot Photovoltaics by Graphene Incorporated into ZnO Nanoparticles.

Single-layer graphene (SLG) was incorporated into ZnO nanoparticles (NPs), and use of this material in photovoltaic devices generated significant changes. The Fermi level of ZnO NPs underwent a downshift, whereas the conduction and valence bands were maintained with increasing SLG concentrations. Furthermore, the effective defect densities were reduced and carrier mobility was enhanced. Colloidal quantum dot photovoltaics (CQDPVs) with the SLG-incorporated ZnO NP layer as an electron transporting layer achieved significant performance enhancement. Poor performing CQDPVs were also observed with incorporation of an excess amount of SLG. This trend paralleled the interfacial charge recombination trends of CQDPVs. Effective suppression of interfacial recombination was achieved for CQDPVs with an appropriate SLG concentration, whereas dramatically increased interfacial recombination was observed for CQDPVs with an excess of SLG. For CQDPVs with appropriate SLG incorporation, efficient defect passivation and enhanced electron mobility of ZnO NPs facilitated loss-less electron transfer and efficient electron extraction without compromising the favorable energy level alignment. Excess SLG incorporation led to an increase in recombination within the PbS QD layer due to the presence of an energy barrier. This simple and powerful strategy provides an effective method for modulating the interfacial properties of CQDPVs.