Dye-sensitized
solar cells (DSCs) have gained great attention in recent years due
to their low-cost fabrication, flexibility, and high power conversion
efficiency. In a DSC, due to interfaces between the dye and the charge-transport
materials, the interface electrostatics becomes a key factor determining
the overall performance of the cell. Liquid-electrolyte-based DSCs
suffer from low stability, electrolyte leakage, and, in some cases,
electrode corrosion. Replacing liquid electrolyte with a solid semiconducting
material leads to poor interfacial contacts, hence the interface electrostatics
becomes one of the limiting factors. In this work, we present a drift-diffusion
and density functional theory (DFT) study of solid-state DSCs to investigate
the electrostatics at the TiO2/organic dye/Spiro-OMeTAD
interface and its impact on the adsorbed dye energy levels, its absorption
spectrum, and the related charge injection. In our three-dimensional
drift-diffusion model, we solve a set of drift-diffusion equations
coupled to Poisson equation for electrons, holes, doping impurities,
and interface traps simultaneously. After that, we use first-principles
DFT modeling of dye-sensitized interfaces in the presence of the calculated
electric fields. We find that interface traps located below the conduction
band edge of mesoporous TiO2 influence the accumulation
of photogenerated holes and built-in electric field near the interface.
The built-in electric field leads to change in the energetics at the
dye/TiO2 interface, leading to poor charge injection from
excited dye into TiO2. The simulations were carried out
for different electronic trap densities in TiO2 and different
doping levels in the Spiro-OMeTAD hole-transport layer. This study
helps to a better understanding of the interface electrostatics and
its role in the charge injection mechanism of solid-state DSCs.