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Two-dimensional layered semiconductors have attracted intense interest in recent years. The van der Waals coupling between the layers tolerates stacking various materials and establishing heterostructures with new characteristics for a wide range of optoelectronic applications. The interlayer exciton dynamics at the interface within the heterostructure are vitally important for the performance of the photodetector and photovoltaic device. Here, a heterostructure comprising two-dimensional organic-inorganic Ruddlesden–Popper perovskites and transition metal dichalcogenide monolayer was fabricated and its ultrafast charge separation processes were systematically studied by using femtosecond time-resolved transient absorption spectroscopy. Significant hole and electron transfer processes in the ps and fs magnitude at the interface of the heterostructure were observed by tuning pump wavelengths of the pump-probe geometries. The results emphasize the realization of the exciton devices based on semiconductor heterostructures of two-dimensional perovskite and transition metal dichalcogenide.

The quasi-2D Dion–Jacobson perovskite exhibits significant photophysical properties and potential applications. However, the insufficient exciton energy transfer leads to nonradiative recombination that seriously hinders charge transport. Here, an efficient energy transfer is achieved by incorporating the alkali metal, which not only constrains the nucleation of high-n phases and promotes the growth of the middle-n phases but also optimizes the phase distribution and the crystal orientation to promote carrier transport. We achieve a green amplified spontaneous emission with a low threshold of 28.5 μJ/cm2 and a vertical-cavity laser operating in a single-mode configuration with a linewidth of 0.96 nm. [ABSTRACT FROM AUTHOR]

Quasi-2D Dion–Jacobson (DJ) halide perovskites with large exciton binding energy, self-assembled quantum wells, and high quantum yield attract growing attention in light-emitting diodes and solar devices. DJ-layered perovskites have the eliminated van der Waals gap and show improved photophysical features. However, there are a variety of defects and complex phase distributions produced during the solution procedure and the fast crystal development. In this paper, we reveal the effect of phase distribution and defect passivation on amplified spontaneous emission of quasi-2D perovskite (PDMA)(MA)2Pb3Br10 thin films through solvent engineering and additive methods, by establishing the correlation between the precursor compositions and the photophysical performance of the layered DJ perovskites. The energy transfer rate and the photoluminescence quantum yield increase due to the spatially homogeneous domain distribution and the reduced defect density after the addition of KBr in the DMSO:DMF. More importantly, we realize green amplified spontaneous emission and single-mode vertical-cavity surface-emitting lasing with low thresholds of 8.8 and 10.5 μJ cm−2, respectively. This work provides a guideline to achieve low-threshold multicolor lasers based on DJ perovskites. [ABSTRACT FROM AUTHOR]

Two-dimensional layered semiconductors have attracted intense interest in recent years. The van der Waals coupling between the layers tolerates stacking various materials and establishing heterostructures with new characteristics for a wide range of optoelectronic applications. The interlayer exciton dynamics at the interface within the heterostructure are vitally important for the performance of the photodetector and photovoltaic device. Here, a heterostructure comprising two-dimensional organic-inorganic Ruddlesden–Popper perovskites and transition metal dichalcogenide monolayer was fabricated and its ultrafast charge separation processes were systematically studied by using femtosecond time-resolved transient absorption spectroscopy. Significant hole and electron transfer processes in the ps and fs magnitude at the interface of the heterostructure were observed by tuning pump wavelengths of the pump-probe geometries. The results emphasize the realization of the exciton devices based on semiconductor heterostructures of two-dimensional perovskite and transition metal dichalcogenide. [ABSTRACT FROM AUTHOR]