Transition metal dichalcogenide (TMDCs) monolayers make an excellent component in optoelectronic devices such as photodetectors and phototransistors. Selenide‐based TMDCs, specifically molybdenum diselenide (MoSe2) monolayers with low defect densities, show much faster photoresponses compared to their sulfide counterpart. However, the typically low absorption of the atomically thin MoSe2 monolayer and high exciton binding energy limit the photogeneration of charge carriers. Yet, integration of light‐harvesting materials with TMDCs can produce increased photocurrents via energy transfer. In this article, it is demonstrated that the interaction of cesium lead bromide (CsPbBr3) nanocrystals with MoSe2 monolayers results into an energy transfer efficiency of over 86%, as ascertained from the quenching and decay dynamics of the CsPbBr3 nanocrystals emission. Notably, the increase in the MoSe2 monolayer emission in the heterostructure accounts only for 33% of the transferred energy. It is found that part of the excess energy generates directly free carriers in the MoSe2 monolayer, as a result of the transfer of energy into the exciton continuum. The efficiency of the heterostructure via enhanced photocurrents with respect to the single material unit is proven. These results demonstrate a viable route to overcome the high exciton binding energy typical for TMDCs, as such having an impact on optoelectronic processes that rely on efficient exciton dissociation.

Nowadays, as a result of the emergence of low-dimensional hybrid structures, the scientific community is interested in their interfacial carrier dynamics, including charge transfer and energy transfer. By combining the...

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Cesium lead bromide (CsPbBr3) nanocrystals with excellent absorption and emission properties when coupled to a molybdenum diselenide (MoSe2) monolayer, transfer more than 86% of their photo‐excited energy to MoSe2. As a result, shown by Ilka Kriegel and co‐workers in article number 2200638, enhancement of MoSe2 emission can be observed, but most of the transferred energy results in the generation of free carriers in MoSe2. [Cover art by Andrea Rubino.]