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Interface engineering of organic-inorganic halide perovskite solar cells(PSCs) plays a pivotal role in achieving high power conversion efficiency(PCE). Graphene and related two-dimensional materials (GRMs) are promisingcandidates to tune on demand the interface properties of PSCs. In this work, wefully exploit the potential of GRMs by controlling the optoelectronicproperties of hybrids between molybdenum disulfide (MoS2) and reduced grapheneoxide (RGO) as hole transport layer (HTL) and active buffer layer (ABL) inmesoscopic methylammonium lead iodide (CH3NH3PbI3) perovskite (MAPbI3)-basedPSC. We show that zero-dimensional MoS2 quantum dots (MoS2 QDs), derived byliquid phase exfoliated MoS2 flakes, provide both hole-extraction andelectron-blocking properties. In fact, on the one hand, intrinsic n-typedoping-induced intra-band gap states effectively extract the holes through anelectron injection mechanism. On the other hand, quantum confinement effectsincrease the optical band gap of MoS2 (from 1.4 eV for the flakes to > 3.2 forQDs), raising the minimum energy of its conduction band (from -4.3 eV for theflakes to -2.2 eV for QDs) above the one of conduction band of MAPbI3 (between-3.7 and -4 eV) and hindering electron collection. The van der Waalshybridization of MoS2 QDs with functionalized reduced graphene oxide (f-RGO),obtained by chemical silanization-induced linkage between RGO and(3-mercaptopropyl)trimethoxysilane, is effective to homogenize the depositionof HTLs or ABLs onto the perovskite film, since the two-dimensional (2D) natureof RGO effectively plug the pinholes of the MoS2 QDs films. Our grapheneinterface engineering (GIE) strategy based on van der Waals MoS2 QD/graphenehybrids enable MAPbI3-based PSCs to achieve PCE up to 20.12% (average PCE of18.8%).

MoS2 Quantum Dot/Graphene Hybrids for Advanced Interface Engineering of CH3NH3PbI3 Perovskite Solar Cell with Efficiency over 20%