The hot-phonon bottleneck effect in lead-halide perovskites (APbX3) prolongs the cooling period of hot charge carriers, an effect that could be used in the next-generation photovoltaics devices. Using ultrafast optical characterization and first-principle calculations, four kinds of lead-halide perovskites (A=FA+/MA+/Cs+, X=I−/Br−) are compared in this study to reveal the carrier-phonon dynamics within. Here we show a stronger phonon bottleneck effect in hybrid perovskites than in their inorganic counterparts. Compared with the caesium-based system, a 10 times slower carrier-phonon relaxation rate is observed in FAPbI3. The up-conversion of low-energy phonons is proposed to be responsible for the bottleneck effect. The presence of organic cations introduces overlapping phonon branches and facilitates the up-transition of low-energy modes. The blocking of phonon propagation associated with an ultralow thermal conductivity of the material also increases the overall up-conversion efficiency. This result also suggests a new and general method for achieving long-lived hot carriers in materials.
Silicon (Si) quantum dot (QD) materials have been proposed for 'all-silicon' tandem solar cells. In this study, solar cells consisting of phosphorus-doped Si QDs in a SiO(2) matrix deposited on p-type crystalline Si substrates (c-Si) were fabricated. The Si QDs were formed by alternate deposition of SiO(2) and silicon-rich SiO(x) with magnetron co-sputtering, followed by high-temperature annealing. Current tunnelling through the QD layer was observed from the solar cells with a dot spacing of 2 nm or less. To get the required current densities through the devices, the dot spacing in the SiO(2) matrix had to be 2 nm or less. The open-circuit voltage was found to increase proportionally with reductions in QD size, which may relate to a bandgap widening effect in Si QDs or an improved heterojunction field allowing a greater split of the Fermi levels in the Si substrate. Successful fabrication of (n-type) Si QD/(p-type) c-Si photovoltaic devices is an encouraging step towards the realization of all-silicon tandem solar cells based on Si QD materials.