Gigantic suppression of recombination rate in 3D lead-halide perovskites for enhanced photodetector performance

Prolonging the carrier lifetime in lead-halide perovskite (LHP) can enable novel schemes for highly efficient energy-harvesting and photodetection applications. However, suppressing the recombination processes in LHP without chemical treatments remains an open challenge. Here we show that the recombination rate of three-dimensional LHP polycrystalline thin films can decrease significantly when placed on hyperbolic metamaterials. Through momentum-resolved imaging, we reveal that these LHP films possess a dominant in-plane transition dipole, which in turn is responsible for the decrease in the recombination rate. We observe a decrease in the recombination rate of a MAPbI(3) LHP thin film by similar to 50% and 30% when placed on a plasmonic mirror and a hyperbolic metamaterial, respectively. Furthermore, we discover a tenfold decrease in the recombination rate of (Cs(0.06)FA(0.79)MA(0.15))Pb(I0.85Br0.15)(3), and the origin of this giant reduction in the recombination process is discussed based on exciton-trapping dynamics. By controlling the recombination rate of LHPs, we demonstrate a 250% increase in photoresponsivity of LHP-based photodetectors. The resulting physical insights will provide novel means to enhance the efficiency of LHP-based optoelectronic and photonic devices.

Automated summary

Placing three-dimensional lead-halide perovskite films on hyperbolic metamaterials can significantly decrease the recombination rate and prolong the carrier lifetime. This decrease is attributed to the dominant in-plane transition dipole of the films. The insights gained from this study offer novel means to enhance the efficiency of perovskite-based optoelectronic and photonic devices.