Vapor-Phase Formation of a Hole-Transporting Thiophene Polymer Layer for Evaporated Perovskite Solar Cells.

Homogeneous layer formation on textured silicon substrates is essential for the fabrication of highly efficient monolithic perovskite silicon tandem solar cells. From all well-known techniques for the fabrication of perovskite solar cells (PSCs), the evaporation method offers the highest degree of freedom for layer-by-layer deposition independent of the substrate's roughness or texturing. Hole-transporting polymers with high hole mobility and structural stability have been used as effective hole-transporting materials (HTMs) of PSCs. However, the strong intermolecular interactions of the polymers do not allow for a layer formation via the evaporation method, which is a big challenge for the perovskite community. Herein, we first applied a hole-transporting terthiophene polymer (PTTh) as an HTM for evaporated PSCs via an in situ vapor-phase polymerization using iodine (I2) as a sublimable oxidative agent. PTTh showed high hole mobility of 1.2 × 10-3 cm2/(V s) and appropriate energy levels as HTM in PSCs (EHOMO = -5.3 eV and ELUMO = -3.3 eV). The PSCs with the in situ vapor-phase polymerized PTTh hole-transporting layer and a co-evaporated perovskite layer exhibited a photovoltaic conversion efficiency of 5.9%, as a proof of concept, and high cell stability over time. Additionally, the polymer layer could fully cover the pyramidal structure of textured silicon substrates and was identified as an effective hole-transporting material for perovskite silicon tandem solar cells by optical simulation.

Anti-Oxidizing Radical Polymer-Incorporated Perovskite Layers and their Photovoltaic Characteristics in Solar Cells.

A small amount of a radical-bearing redox-active polymer, poly(1-oxy-2,2,6,6-tetramethylpiperidin-4-yl methacrylate) (PTMA), incorporated into the photovoltaic organo-lead halide perovskite layer significantly enhanced durability of both the perovskite layer and its solar cell and even exposure to ambient air or oxygen. PTMA acted as an eliminating agent of the superoxide anion radical formed upon light irradiation on the layer, which can react with the perovskite compound and decompose it to lead halide. A cell fabricated with a PTMA-incorporated perovskite layer and a hole-transporting polytriarylamine layer gave a photovoltaic conversion efficiency of 18.8 % (18.2 % for the control without PTMA). The photovoltaic current was not reduced in the presence of PTMA in the perovskite layer probably owing to a carrier conductivity of PTMA. The incorporated PTMA also worked as a water-repelling coating for providing humidity-resistance to the organo-lead halide perovskite layer.