Dye-sensitized solar cells (DSSCs) are a promising third-generation photovoltaic cell technology whose advantages are low-cost fabrication, reduced energy payback time, better performance under diffuse light conditions and flexibility. Typically DSSCs employ toxic dyes such as metal-based porphyrins requiring complex synthesis. In contrast, natural pigments are environmentally and economically superior to synthetic dyes. However, narrow absorption spectra of natural pigments result in low efficiencies of the solar cells. Hence, co-sensitizing pigments with complementary absorption spectra, which increases the absorption band, is an attractive pathway to enhance the efficiency. In this paper, we report the performance of betanin-chlorophyll co-sensitized solar cell using betanin (λ max = 535 nm) and chlorophyll-a (λ max = 435 nm, 668 nm), natural pigments having complementary absorption spectra. Density functional theory simulations were performed to verify that the lowest unoccupied molecular orbital and the highest occupied molecular orbital levels of the dye molecules, are aligned appropriately with that of TiO 2 and the redox electrolyte, respectively, which is necessary for optimal device performance. Electrochemical impedance spectroscopic studies were performed to determine parameters corresponding to the charge transfer processes in the dye solar cells. Individual and co-sensitized solar cells were fabricated and the co-sensitized solar cell demonstrated a higher efficiency of 0.601% compared to efficiencies of 0.562% and 0.047% shown by betanin and chlorophyll solar cells, respectively.

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. Since the seminal work in 1991 by O'Regan and Gratzel on Dye-Sensitized Solar Cells (DSSCs) 1 , immense interest has been directed towards their development in the last two decades. Owing to their inexpensive and facile processing requirements, DSSCs are becoming increasingly popular as an emerging photovoltaic technology 2-4. State-of-the-art DSSCs, which have achieved maximum efficiencies of 11.9% 5 , widely use metal-based dyes as the photosensitizer. Although these dyes are highly efficient sensitizers that effectively capture the entire visible spectrum, they employ rare metals such as ruthenium or osmium which require elaborate synthetic procedures. Moreover, they are expensive and toxic to the environment, making their disposal a problem. Therefore, natural pigments derived from plant sources, which are environment-friendly and inexpensive 6,7 , have come to the forefront as alternative photosensitizers. Several groups 8,...

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Co-sensitization is an important strategy toward efficiency enhancement of solar cells by enabling better light harvesting across the solar spectrum. Betanin is a natural dye which absorbs light in the major portion of the incident solar spectrum (green region) and is the most efficient natural pigment used in dye-sensitized solar cells. This study investigates the performance enhancement of a betanin solar cell by co-sensitizing it with two natural pigments which show complementary light absorption, i.e., indigo and lawsone, absorbing in the red and blue regions of the solar spectrum, respectively. The calculated highest occupied molecular orbital and lowest unoccupied molecular orbital energies of the pigment molecules, derived from density functional theory (DFT) simulations, confirmed their optimal alignment with respect to the conduction band energy of the TiO2 semiconductor and reduction potential energy level of the I–/I3– electrolyte, a necessary requirement for optimal device performance. Lawsone solar cells displayed better performance, showing average efficiencies of 0.311 ± 0.034%, compared to indigo solar cells showing efficiencies of 0.060 ± 0.004%. Betanin was co-sensitized with indigo and lawsone, and the performances of the co-sensitized solar cells were compared. The betanin/lawsone co-sensitized solar cell showed a higher average efficiency of 0.793 ± 0.021% compared to 0.655 ± 0.019% obtained for the betanin/indigo co-sensitized solar cell. An 11.7% enhancement in efficiency (with respect to betanin) was observed for the betanin/indigo solar cell, whereas a higher enhancement of 25.5% was observed for the betanin/lawsone solar cell. Electrochemical impedance spectroscopy studies confirmed that the higher efficiency can be attributed to the higher electron lifetime of 313.8 ms in the betanin/lawsone co-sensitized solar cell compared to 291.4 ms in the betanin/indigo solar cell. This is due to the energy levels being more optimally aligned in lawsone compared to that of indigo, as observed in the DFT studies, and the lack of dipole moment in indigo, resulting in more efficient charge separation and charge transfer in lawsone.

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