Enhancement of Spectral Response of Dye-Sensitized Solar Cells

Dye-Sensitized solar cell (DSSC) is a class of third-generation solar devices. A notable feature of DSSC is that it can be manufactured by solution-based approach; this non-vacuum processing renders significant reduction in manufacturing costs. Different from conventional solar cells, in a DSSC, mesoporous semiconductor film with large surface areas is utilized for anchoring dye molecules, serving as light absorbing layer.;Dye sensitizers play an important role in determining the final performance in DSSCs. Since the first highly-efficient DSSC was reported in 1991 sensitized by a ruthenium-based dye, numerous researchers have been focused on the development and characterization of various kinds of dyes for the applications in DSSCs. These include mainly metal complexes dyes, organic dyes, porphyrins and phthalocyanines dyes. The first part of my thesis work is to develop and test new dyes for DSSCs and a series of phenothiazine-based organic dyes and new porphyrin dyes are reported during the process.;It has been realized that extending the response of dye sensitizers to a wider range of the solar spectrum is a key step in further improving the device efficiency. Typically, there are two ways for expanding the strong spectral response of DSSCs from visible to far red/NIR region.;One approach is called co-sensitization. Herein, we demonstrate a new co-sensitization concept where small molecules is used to insert the interstitial site of between the pre-adsorbed large molecules. In this case, the co-adsorbed small ones is found to improve the light response and impede the back recombination, finally leading to the power conversion efficiency over 10% in conventional DSSC devices and a record-equaling efficiency of 9.2% in quasi-solid-state devices. I also implemented graphene sheets in the anode films for better charge transfer efficiency and break the energy conversion limit of co-sensitization in DSSCs. The optimal configuration between porphyrin dyes and ruthenium-based/organic dyes for co-sensitized DSSCs are also investigated.;Another approach is to increase light utility in DSSCs exploiting surface plasmon resonance (SPR) of noble metal nanostructures (e.g. Au, Ag). In this thesis, I will show that the strong longitudinal plasmonic absorption of Au nanorods (NRs) can be used to increase the low-photon energy sunlight harvesting in DSSCs, broadening strong light response of the devices. In specific, a remarkable improvement in photocurrent generation at 600-720 nm is achieved. This enhancement mechanism is anticipated to be applied to other kind of DSSCs with various dye molecules. In another approach, AuNRs/TiO2 core-shell nanostructures are employed as scattering layer for plasmon-enhanced light harvesting in DSSCs and also obtained positive results.;Evolved from DSSCs, perovskite solar cells (PSCs) now become a new favorite in the field of photovoltaics. An intrinsic problem of this kind of solar cells is the use of lead based materials, which is of high toxicity and prohibited by the European Union and some other countries. I have conducted some fundamental research for lead-free PSCs using tin-based perovskite and have observed a surface plasmon resonance absorption of the organometal perovskite film of CH3NH3SnI3, which has potential applications for IR-absorption in the future solar photovoltaics.;I believe the improved understanding on the co-sensitization mechanisms and the plasmonic effect to broaden the spectral response in DSSCs are luciferous for the design and fabrication of the new generation solar cells with high-efficiency and low-cost.