Surface plasmon-mediated photoluminescence boost in graphene-covered CsPbBr$_3$ quantum dots

Abstract: The optical properties of graphene (Gr)-covered CsPbBr$_3$ quantum dots (QDs) were investigated using micro-photoluminescence spectroscopy, revealing a remarkable three-orders-of-magnitude enhancement in photoluminescence (PL) intensity compared to bare CsPbBr$_3$ QDs. To elucidate the underlying mechanisms, we combined experimental techniques with density functional theory (DFT) calculations. DFT simulations showed that the graphene layer generates interfacial electrostatic potential barriers when in contact with the CsPbBr$_3$ surface, impeding carrier leakage from perovskite to graphene and enhancing radiative recombination. Additionally, graphene passivates CsPbBr$_3$ surface defect states, suppressing nonradiative recombination of photo-generated carriers. Our study also revealed that graphene becomes n-doped upon contact with CsPbBr$_3$ QDs, activating its plasmon mode. This mode resonantly couples with photo-generated excitons in the perovskite. The momentum mismatch between graphene plasmons and free-space photons is resolved through plasmon scattering at Gr/CsPbBr$_3$ interface corrugations, facilitating the observed super-bright emission. These findings highlight the critical role of graphene as a top contact in dramatically enhancing CsPbBr$_3$ QDs' PL. Our work advances the understanding of graphene-perovskite interfaces and opens new avenues for designing high-efficiency optoelectronic devices. The multifaceted enhancement mechanisms uncovered provide valuable insights for future research in nanophotonics and materials science, potentially leading to breakthroughs in light-emitting technologies.