Flexible semitransparent perovskite solar cells with gradient energy levels enable efficient tandems with Cu(In,Ga)Se2

Flexible semitransparent perovskite solar cells (PVSCs) hold promising applications on buildings and unmanned vehicles with irregular surfaces. Efficient wide-bandgap PVSCs are a determining factor for building perovskite-based tandem cells, in which energy level alignment plays significant roles in reducing nonradiative recombination loss at interfaces. Here, we report on the fabrication of efficient flexible semitransparent wide-bandgap PVSCs with gradient energy level alignments at both electron- and hole-selective contacts. We design a triple-electron-selective contact as electron transport layers with gradient Fermi level alignment with the conduction band of wide-bandgap perovskite, which consists of trans-1,2-Diaminocyclohexane-N,N,N′,N′-tetraacetic (CyDTA), tin dioxide (SnO2), and CyDTA-complexed SnO2. Moreover, an ultrathin gold layer embedded between 2,2′,7,7′-tetrakis(N,N-bis(p-methoxy-phenyl)amino)-9,9′-spirobifluorene (spiro-OMeTAD) hole transport layer and molybdenum oxide protection layer facilitates effective hole transport to the anode. We conduct comprehensive and solid simulation at both charge-selective contacts to reveal the working mechanisms. The champion flexible semitransparent 1.75 eV wide-bandgap PVSC achieves an efficiency of 15.02% with excellent light transparency of around 70% beyond the wavelength of 700 nm, enabling all-flexible perovskite/Cu(In,Ga)Se2 tandem devices with efficiencies beyond 21%.