Abstract

Organic–inorganic metal halide perovskites (MHPs) have recently been receiving a lot of attention due to their newfound application in optoelectronic devices, including perovskite solar cells (PSCs) which have reached power conversion efficiencies as high as 25.5%. However, the fundamental mechanisms in PSCs, including the correlation of degradation with the excellent optoelectrical properties of the perovskite absorbers, are poorly understood. In this paper, we have explored synchrotron-based soft X-ray characterization as an effective technique for the compositional analysis of MHP thin films. Most synchrotron-based studies used for investigating MHPs so far are based on hard X-rays (5–10 keV) which include various absorption edges (Pb L-edge, I L-edge, Br K-edge, etc.) but are not suited for the analysis of the organic component in these materials. In order to be sensitive to a maximum number of elements, we have employed soft X-ray-based scanning transmission X-ray microscopy (STXM) as a spectro-microscopy technique for the characterization of MHPs. We examined its sensitivity to iodine and organic components, aging, or oxidation by-products in MHPs to make sure that our suggested method is suitable for studying MHPs. Furthermore, methylammonium triiodide with different deposition ratios of PbI2 and CH3NH3I (MAI), and different thicknesses, were characterized for chemical inhomogeneity at the nanoscale by STXM. Through these measurements, we demonstrate that STXM is very sensitive to chemical composition and homogeneity in MHPs. Thus, we highlight the utility of STXM for an in-depth analysis of physical and chemical phenomena in PSCs.

Highlights

  • Organic–inorganic metal halide perovskites (MHPs) have recently been receiving a lot of attention due to their newfound application in optoelectronic devices, including perovskite solar cells (PSCs) which have reached power conversion efficiencies as high as 25.5%

  • In comparison to the simulated spectrum, the experimental MAI spectrum appears with an inhibited I M-edge. This fact is supported by energy-dispersive X-ray spectroscopy (EDX) analysis of MAI films (Fig. S1 and Table S1), wherein the iodine atomic percent was observed to be small compared with those of carbon and nitrogen

  • We highlight the utility of scanning transmission X-ray microscopy (STXM) in the soft X-ray regime to characterize organic–inorganic MHPs

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Summary

Introduction

Organic–inorganic metal halide perovskites (MHPs) have recently been receiving a lot of attention due to their newfound application in optoelectronic devices, including perovskite solar cells (PSCs) which have reached power conversion efficiencies as high as 25.5%. The X-ray absorption spectrum of PbO obtained from STXM is measured to identify the by-product issued from the degradation of ­MAPbI3 (MHP in this study). ­MAPbI3 samples with different ­PbI2:MAI ratios and of various thicknesses were prepared and compared to highlight the chemical and thickness sensitivity of STXM.

Results
Conclusion
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