Band Structure Engineering of Interfacial Semiconductors Based on Atomically Thin Lead Iodide Crystals

To explore new constituents in two-dimensional materials and to combine their best in van der Waals heterostructures, are in great demand as being unique platform to discover new physical phenomena and to design novel functionalities in interface-based devices. Herein, PbI2 crystals as thin as few-layers are first synthesized, particularly through a facile low-temperature solution approach with the crystals of large size, regular shape, different thicknesses and high-yields. As a prototypical demonstration of flexible band engineering of PbI2-based interfacial semiconductors, these PbI2 crystals are subsequently assembled with several transition metal dichalcogenide monolayers. The photoluminescence of MoS2 is strongly enhanced in MoS2/PbI2 stacks, while a dramatic photoluminescence quenching of WS2 and WSe2 is revealed in WS2/PbI2 and WSe2/PbI2 stacks. This is attributed to the effective heterojunction formation between PbI2 and these monolayers, but type I band alignment in MoS2/PbI2 stacks where fast-transferred charge carriers accumulate in MoS2 with high emission efficiency, and type II in WS2/PbI2 and WSe2/PbI2 stacks with separated electrons and holes suitable for light harvesting. Our results demonstrate that MoS2, WS2, WSe2 monolayers with very similar electronic structures themselves, show completely distinct light-matter interactions when interfacing with PbI2, providing unprecedent capabilities to engineer the device performance of two-dimensional heterostructures.Comment: 36 pages, 5 figure

Efficient inverted perovskite solar cells via improved sequential deposition

Inverted-structure metal halide perovskite solar cells (PSCs) have attractive advantages like low-temperature processability and outstanding device stability. The two-step sequential deposition method shows the benefits of easy fabrication and decent performance repeatability. Nevertheless, it is still challenging to achieve high-performance inverted PSCs with similar or equal power conversion efficiencies (PCEs) compared to the regular-structure counterparts via this deposition method. Here, an improved two-step sequential deposition technique is demonstrated via treating the bottom organic hole-selective layer with the binary modulation system composed of a polyelectrolyte and an ammonium salt. Such improved sequential deposition method leads to the spontaneous refinement of up and buried interfaces for the perovskite films, contributing to high film quality with significantly reduced defect density and better charge transportation. As a result, the optimized PSCs show a large enhancement in the open-circuit voltage by 100 mV and a dramatic lift in the PCE from 18.1% to 23.4%, delivering the current state-of-the-art performances for inverted PSCs. Moreover, good operational and thermal stability is achieved upon the improved inverted PSCs. This innovative strategy helps gain a deeper insight into the perovskite crystal growth and defect modulation in the inverted PSCs based on the two-step sequential deposition method