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.