In this study, the spontaneous microstructure tuning of TiO2 was observed by aging the ethanol/water TiO2 paste for up to 20 days at ambient conditions. A dynamic light scattering study reveals that it formed the outstanding reproducible TiO2 microstructure with a ∼200 nm average particle size and stabilizes in 6 to 20 days under an ambient atmosphere. Interestingly, the as-deposited day 15 sample spontaneously changed its crystallinity upon keeping the paste at ambient conditions; meanwhile the day 0 sample showed an amorphous structure. A dense, uniform, and stable TiO2 electrode was cast on a fluorine doped-tin oxide substrate using the electrospray technique. We exploit the spontaneous evolution of the TiO2 nanopowder to revisit the fabrication procedure of the TiO2 photoelectrode for dye-sensitized solar cells (DSSCs). The controlled microstructure TiO2 film was used in DSSCs, which, to the best of our knowledge, achieved the highest power conversion efficiency of 9.65% using N719 dye in sensitizing the TiO2 photoanode.
The photovoltaic performance of perovskite solar cells (PSCs) can be improved by utilizing efficient front contact. However, it has always been a significant challenge for fabricating high-quality, scalable, controllable, and cost-effective front contact. This study proposes a realistic multi-layer front contact design to realize efficient single-junction PSCs and perovskite/perovskite tandem solar cells (TSCs). As a critical part of the front contact, we prepared a highly compact titanium oxide (TiO2) film by industrially viable Spray Pyrolysis Deposition (SPD), which acts as a potential electron transport layer (ETL) for the fabrication of PSCs. Optimization and reproducibility of the TiO2 ETL were discreetly investigated while fabricating a set of planar PSCs. As the front contact has a significant influence on the optoelectronic properties of PSCs, hence, we investigated the optics and electrical effects of PSCs by three-dimensional (3D) finite-difference time-domain (FDTD) and finite element method (FEM) rigorous simulations. The investigation allows us to compare experimental results with the outcome from simulations. Furthermore, an optimized single-junction PSC is designed to enhance the energy conversion efficiency (ECE) by > 30% compared to the planar reference PSC. Finally, the study has been progressed to the realization of all-perovskite TSC that can reach the ECE, exceeding 30%. Detailed guidance for the completion of high-performance PSCs is provided.