New indole based co-sensitizers for dye sensitized solar cells exceeding 10% efficiency

In this work, we report the molecular engineering and synthesis of three novel indole co-sensitizers DBA-3, DBA-4 and DBA-5 with D–D–A (donor–donor–acceptor) architecture. In the quest to comprehend the role of auxiliary donors on co-sensitization, we have incorporated auxiliary electron donating moieties with varying geometries and electron donating capabilities to the indole moiety in order to obtain the aforementioned co-sensitizers. Their electrochemical and photo-physical properties along with molecular geometries, obtained from Density Functional Theory (DFT) are studied to vindicate the effect of the co-sensitizer structures on the photovoltaic properties of DSSCs. Furthermore, for the first time we demonstrate the profound effect of auxiliary donor groups on the co-sensitization performance of the organic molecules. Devices co-sensitized using DBA-3, DBA-4 and DBA-5 along with ruthenium sensitizer NCSU-10, displayed significantly different photovoltaic conversion efficiencies (PCEs) when compared to that of the device sensitized using only NCSU-10. The photovoltaic and EIS studies revealed that, the co-sensitizer DBA-4 succeeded in enhancing the light harvesting capability as well as efficiently suppressing undesirable charge recombinations in the cell. Due to the aforementioned reasons, a cell co-sensitized using DBA-4 has shown promising photovoltaic results and exhibited an enhanced overall efficiency of 10.12%. Furthermore, vertical electronic excitations, calculated using TD-DFT, are in good agreement with the experimental λₘₐₓ results, which clearly indicates that, the energy functional and basis set utilized in this study can be effectively employed for predicting the absorption spectra of novel photosensitizers, with high confidence prior to their synthesis. All these results provide a better understanding and deeper insight into the intricacies involved in the design of superior co-sensitizers to further improve the performance of DSSCs.