نبذة مختصرة : Natural pigment-based photosensitizers are an attractive pathway for realizing low cost and environmentally friendly solar cells. Here, broadband light-harvesting is achieved using two natural pigments, betanin and lawsone, absorbing in the green and blue region of the solar spectrum respectively. The use of bimodal size distribution of AgNPs tailored for each of the pigments to further increase their efficiency is the key feature of this work. This study demonstrates a significant enhancement in current-density, voltage, and efficiency by 20.1%, 5.5%, and 28.6% respectively, in a betanin-lawsone co-sensitized solar cell, via plasmonic enhancement using silver nanoparticles (AgNPs). The optimum sizes of the nanoparticles have been calculated by studying their optical response and electric field profiles using Finite Difference Time Domain (FDTD) simulations, aimed at matching their resonant wavelengths with the absorption bands of the dyes. Simulations show that AgNPs of diameters 20 nm and 60 nm are optimum for enhanced absorption by lawsone and betanin respectively. The FDTD simulations of the plasmonic photoelectrodes demonstrated 30% and 15% enhancement in the power absorption by betanin and lawsone at the LSPR peaks of the 60 nm and 20 nm AgNPs respectively. An optimum overall concentration of 2% (v/v) and a ratio of 4:1 (20 nm:60 nm) of the bimodal distribution of the AgNPs, was determined for incorporation in the photoanodes. An average efficiency of 1.02 ± 0.006% was achieved by the betanin-lawsone co-sensitized solar cell with the bimodal distribution of AgNPs, compared to 0.793 ± 0.006% achieved by the non-plasmonic solar cell of otherwise identical configuration. Electrochemical impedance spectroscopy confirmed that the incorporation of the bimodal distribution of AgNPs in the solar cells also enabled enhanced electron lifetime and reduced recombination compared to the non-plasmonic counterpart, thereby improving the charge transfer. The plasmonic enhancement methodology presented here can be applied to further improve the efficiency of other natural dye-sensitized solar cells.
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