Surface plasmon-mediated photoluminescence boost in graphene-covered CsPbBr3 quantum dots

Abstract

The optical properties of graphene (Gr)-covered CsPbBr₃ quantum dots (QDs) were investigated using micro-photoluminescence spectroscopy, revealing a remarkable three orders of magnitude enhancement in photoluminescence (PL) intensity compared to bare CsPbBr₃ 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 CsPbBr₃ surface, impeding carrier leakage from perovskite to graphene and enhancing radiative recombination. Additionally, graphene passivates CsPbBr₃ surface defect states, suppressing nonradiative recombination of photo-generated carriers. Our study also revealed that graphene becomes n-doped upon contact with CsPbBr₃ 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/CsPbBr₃ interface corrugations, facilitating the observed super-bright emission. These findings highlight the critical role of graphene as a top contact in dramatically enhancing CsPbBr₃ 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.