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Engineered Interfacial Control for Suppression of Phase Instability: Operando Visualization from Device to Module

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Summary
This summary is machine-generated.

Phase instability in wide-bandgap perovskite solar cells is linked to poor carrier extraction and defects. Operando spectroscopy reveals degradation starts in inactive areas, guiding stable perovskite photovoltaic design.

Keywords:
deep‐level transient spectroscopy (DLTS)halide phase dynamicsmixed‐halide perovskitesoperando visualizationreal‐time current density–voltage absorption spectroscopy (RTJAS)

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Area of Science:

  • Materials Science
  • Renewable Energy
  • Solid-State Physics

Background:

  • Wide-bandgap mixed-halide perovskites are promising for solar cells but suffer from phase instability, hindering long-term performance.
  • Understanding the origins of this instability is crucial for developing stable perovskite photovoltaic devices.

Purpose of the Study:

  • To visualize and understand the spatially resolved phase evolution in perovskite solar cells under operational bias.
  • To identify the key factors governing phase instability at the device and module scale.

Main Methods:

  • Real-time current density-voltage absorption spectroscopy (RTJAS) with a transparent indium tin oxide top contact for operando, spatially resolved visualization.
  • Deep-level transient spectroscopy (DLTS) and density functional theory (DFT) modeling to analyze interfacial defect landscapes and energetics.
  • Operando RTJAS mapping at the module scale.

Main Results:

  • Phase separation preferentially initiates in regions with insufficient carrier extraction, indicating spatial heterogeneity in phase stability.
  • Interfacial configuration modifications alter phase evolution, linked to differences in defect landscapes and vacancy energetics.
  • Electrically inactive dead areas in monolithic interconnects are preferential sites for phase instability onset.

Conclusions:

  • Phase instability in mixed-halide perovskites is governed by localized charge extraction and interfacial defect energetics.
  • The presented operando RTJAS framework is a diagnostic tool for identifying degradation pathways.
  • Findings offer design guidelines for stable and scalable perovskite photovoltaics from device to module scale.