Electronic coupling between perovskite nanocrystal and fullerene modulates hot carrier capture

Abstract Finding schemes for capturing hot carrier is crucial for designing photovoltaic device that more efficiently converts light into electricity. Currently, utilizing fullerene to enhance the cold electron capture from halide perovskite is remarkably prevalent, however, to date, capturing hot carrier in this system remains unlocked. Here, we demonstrate tuning their electronic coupling drives highly efficient hot carrier capture in inorganic perovskite nanocrystal and fullerene hybrid by transient absorption spectroscopy. The formation of state coupled complexes creates new hot carrier transport channels in their binding sites and reverses the originally forbidden hot carrier capture. Moreover, appropriately controlling phonon bottleneck and Auger heat effects in perovskite nanocrystal is demonstrated to enable more efficient hot carrier capture. Finally, we realizes ~ 84% of maximum hot carrier capture efficiency. The findings advance the modulation of hot carrier dynamics in doner-acceptor heterostructures and are essential for the development of practical hot carrier photovoltaics.