Effect of Zinc-Doping on the Reduction of the Hot-Carrier Cooling Rate in Halide Perovskites

The fast hot-carrier cooling process in the solar-absorbers fundamentally limits their photon-conversion efficiencies. It is highly desirable to develop a solar absorber with long-lived hot-carriers at sun-illumination intensity, which can be used to develop the hot-carrier solar cells with enhanced efficiency. Herein, we reveal that zinc-doped (0.34 %) halide perovskites have the slower hot-carrier cooling compared with the pristine sample through the transient absorption spectroscopy measurements and theoretical calculations. The hot-carrier energy loss rate at the low photoexcitation level of 10¹⁷ cm⁻³ is found to be ≈3 times smaller than that of un-doped perovskites for T=500 K hot carriers, and up to ten times when the hot-carrier temperature approaches the lattice temperature. The incorporation of zinc-dopant into perovskites can reduce the nonadiabatic couplings between conduction bands, which retards the photogenerated hot-carriers relaxation processes. Our findings present a practical strategy to slow down the hot-carrier cooling in perovskites at low carrier densities, which would be invaluable for the further development of practical hot-carrier photovoltaics based on perovskites.