Abstract

Organo-halide perovskite solar cells (PSCs) have emerged as next-generation photovoltaics, owing to their high power-conversion efficiency (PCE), lower production cost, and high flexibility. ABX3-structured methylammonium lead triiodide (CH3NH3PbI3 or MAPbI3) perovskite is a widely studied light-absorbing material in PSCs. Interestingly, a small amount of chlorine incorporation into MAPbI3 increases charge carrier diffusion lengths (from 129 nm to 1069 nm), which enables planar structured PSCs with high PCEs. However, existence of chloride ions in the final perovskite film is still under debate. Contrastingly, few studies reported a negligible amount or absence of chloride ions in the final film, while others reported detection of chloride ions in the final film. Herein, we observed the microstructure and chlorine content of MAPbI3−xClx thin films with increasing temperature via an in-situ nano-Auger spectroscopy and in-situ scanning electron microscopic analysis. The relative precipitation of MAPbI3−xClx films occur at lower temperature and MAPbI3−xClx grains grow faster than those of MAPbI3 grains. Local concentrations of chlorine at intragrain and the vicinity of grain boundary were analyzed to understand the behavior and role of the chloride ions during the microstructural evolution of the MAPbI3−xClx films.

Highlights

  • Organo-halide perovskite (OHP) materials are a hot topic in photovoltaic research due to their excellent light harvesting ability and relatively lower processing costs [1,2,3]

  • Perovskite layers with a composition of MAPbI3−x Clx were prepared on TiO2 layers to make similar conditions for the grain growth of perovskite film that are used for optoelectronic devices, as the surface state of the substrates significantly affects the grain growth behavior

  • The soft baking was performed at 65 ◦ C to remove the solvents or anti-solvents and nucleate the perovskite crystallites

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Summary

Introduction

Organo-halide perovskite (OHP) materials are a hot topic in photovoltaic research due to their excellent light harvesting ability and relatively lower processing costs [1,2,3]. In the past few years, perovskite solar cells (PSCs) have seen tremendous uplift in certified power conversion efficiencies (PCE), less than 14% in 2013 to >25% in 2020 [4,5,6]. ABX3 -structured methylammonium lead halides such as MAPbI3 and MAPbI3−x Clx are the most intensely studied reference materials in PSCs, owing to their remarkable optoelectronic properties [7,8]. The fine control over optoelectronic properties and ease of synthesis has driven MAPbI3 to broad applications, including PSCs [11], solar-water splitting [12], lasing [13], and light-emitting diodes [14]

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