Hybrid Lead-Halide Polyelectrolytes as Interfacial Electron Extraction Layers in Inverted Organic Solar Cells

A series of lead-halide based hybrid polyelectrolytes was prepared and used as interfacial layers in organic solar cells (OSCs) to explore their effect on the energy band structures and performance of OSCs. Nonconjugated polyelectrolytes based on ethoxylated polyethylenimine (PEIE) complexed with PbX₂ (I, Br, and Cl) were prepared as polymeric analogs of the perovskite semiconductors CH₃NH₃PbX₃. The organic/inorganic hybrid composites were deposited onto Indium tin oxide (ITO) substrates by solution processing, and ultraviolet photoelectron spectroscopy (UPS) measurements confirmed that the polyelectrolytes allowed the work function of the substrates to be controlled. In addition, X-ray photoelectron spectroscopy (XPS) results showed that Pb(II) halide complexes were present in the thin film and that the Pb halide species did not bond covalently with the cationic polymer and confirmed the absence of additional chemical bonds. The composite ratio of organic and inorganic materials was optimized to improve the performance of OSCs. When PbBr₂ was complexed with the PEIE material, the efficiency increased up to 3.567% via improvements in open circuit voltage and fill factor from the control device (0.3%). These results demonstrate that lead-halide based polyelectrolytes constitute hybrid interfacial layers which provide a novel route to control device characteristics via variation of the lead halide composition.