Spray Pyrolyzed TiO2 Embedded Multi-Layer Front Contact Design for High-Efficiency Perovskite Solar Cells.

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.

Oblique Electrostatic Inkjet-Deposited TiO2 Electron Transport Layers for Efficient Planar Perovskite Solar Cells.

In this study, a new, simple, and novel oblique electrostatic inkjet (OEI) technique is developed to deposit a titanium oxide (TiO2) compact layer (CL) on fluorine-doped tin oxide (FTO) substrate without the need for a vacuum environment for the first time. The TiO2 is used as electron transport layers (ETL) in planar perovskite solar cells (PSCs). This bottom-up OEI technique enables the control of the surface morphology and thickness of the TiO2 CL by simply manipulating the coating time. The OEI-fabricated TiO2 is characterized tested and the results are compared with that of TiO2 CLs produced by spin-coating and spray pyrolysis. The OEI-deposited TiO2 CL exhibits satisfactory surface coverage and smooth morphology, conducive for the ETLs in PSCs. The power-conversion efficiencies of PSCs with OEI-deposited TiO2 CL as the ETL were as high as 13.19%. Therefore, the present study provides an important advance in the effort to develop simple, low-cost, and easily scaled-up techniques. OEI may be a new candidate for depositing TiO2 CL ETLs for highly efficient planar PSCs, thus potentially contributing to future mass production.

Low-Temperature-Processed Brookite-Based TiO2 Heterophase Junction Enhances Performance of Planar Perovskite Solar Cells.

In the design of electron-transport layers (ETLs) to enhance the efficiency of planar perovskite solar cells (PSCs), facile electron extraction and transport are important features. Here, we consider the effects of different titanium oxide (TiO2) polymorphs, anatase and brookite. We design and fabricate high-phase-purity, single-crystalline, highly conductive, and low-temperature (<180 °C)-processed brookite-based TiO2 heterophase junctions on fluorine-doped tin oxide (FTO) as the substrate. We test and compare single-phase anatase (A) and brookite (B) and heterophase anatase-brookite (AB) and brookite-anatase (BA) as ETLs in PSCs. The power-conversion efficiencies (PCEs) of PSCs with low-temperature-processed single-layer FTO-B as the ETL were as high as 14.92%, which is the highest reported efficiency of FTO-B-based single-layer PSC. This implies that FTO-B serves as an active phase and can be a potential candidate as an n-type ETL scaffold in planar PSCs. Moreover, the surface of highly crystalline brookite TiO2 exhibits a tendency toward interparticle necking, leading to the formation of compact scaffolds. Furthermore, PSCs with heterophase junction FTO-AB ETLs exhibited PCEs as high as 16.82%, which is superior to those of PSCs with single-phase anatase (FTO-A) and brookite (FTO-B) as the ETLs (13.86% and 14.92%, respectively). In addition, the PSCs with FTO-AB exhibited improved efficiency and decreased hysteresis compared with those with FTO-BA (13.45%) due to the suitable band alignment with the perovskite layer, which resulted in superior photogenerated charge-carrier extraction and reduced charge accumulation at the interface between the heterophase junction and perovskite. Thus, the present work presents an effective strategy by which to develop heterophase junction ETLs and manipulate the interfacial energy band to further improve the performance of planar PSCs and enable the clean and eco-friendly fabrication of low-cost mass production.