Abstract

AbstractSolar cells incorporating metal‐halide perovskite (MHP) semiconductors are continuing to break efficiency records for solution‐processed solar cell devices. Scaling MHP‐based devices to larger area prototypes requires the development and optimization of scalable process technology and ink formulations that enable reproducible coating results. It is demonstrated that the power conversion efficiency (PCE) of small‐area methylammonium lead iodide (MAPbI3) devices, slot‐die coated from a 2‐methoxy‐ethanol (2‐ME) based ink with dimethyl‐sulfoxide (DMSO) used as an additive depends on the amount of DMSO and age of the ink formulation. When adding 12 mol% of DMSO, small‐area devices of high performance (20.8%) are achieved. The effect of DMSO content and age on the thin film morphology and device performance through in situ X‐ray diffraction and small‐angle X‐ray scattering experiments is rationalized. Adding a limited amount of DMSO prevents the formation of a crystalline intermediate phase related to MAPbI3 and 2‐ME (MAPbI3‐2‐ME) and induces the formation of the MAPbI3 perovskite phase. Higher DMSO content leads to the precipitation of the (DMSO)2MA2Pb3I8 intermediate phase that negatively affects the thin‐film morphology. These results demonstrate that rational insights into the ink composition and process control are critical to enable reproducible large‐scale manufacturing of MHP‐based devices for commercial applications.

Highlights

  • Metal-halide perovskite (MHP) semiconductors are of interest for various opto-electronic devices: photovoltaics (PV)[1,2,3,4], light-emitting diodes (LED)[5], lasers[6], and photodetectors[7]

  • Through in-depth insight into the film formation process as a function of DMSO content from in-situ X-ray diffraction experiments, we found that just the right amount of DMSO favorably affects thin film growth

  • We were able to achieve highly power conversion efficiency (PCE) of slot-die coated perovskite solar cells reproducibly when just the right amount of DMSO is added to 2-ME based precursor solutions

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Summary

Introduction

Metal-halide perovskite (MHP) semiconductors are of interest for various opto-electronic devices: photovoltaics (PV)[1,2,3,4], light-emitting diodes (LED)[5], lasers[6], and photodetectors[7]. Solvent removal can be facilitated by thermal annealing[14], vacuum[12], gas quenching[15] or the deposition of an anti-solvent, which for larger area samples is often accomplished by dipping into a bath.[16] Currently, the PCE obtained for slot-die coated devices is lower than record device PCEs achieved by spincoating[17] This is due to the fact that there has been considerably less optimization work on SDC for MHP deposition and record-performance spin-coated devices rely on rapid solvent removal and induction of crystallization by deposition of an anti-solvent. We highlight that both the exact amount of DMSO as well as the age of the precursor solution critically affect the coating results and device performance This is critical insight to enable the development of stable and reproducible coating procedures for large scale manufacturing of perovskite solar cell devices. At an optimal content of about 12 mol% DMSO in the 2-ME ink, we demonstrated champion MHP device with efficiency of 20.83%, which is among the highest value reported in slot-die coated PSCs

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