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Two-dimensional transition metal dichalcogenides (TMDCs) have recentlyattracted attention due to their superlative optical and electronic properties.In particular, their extraordinary optical absorption and semiconducting bandgap have enabled demonstrations of photovoltaic response from heterostructurescomposed of TMDCs and other organic or inorganic materials. However, theseearly studies were limited to devices at the micrometer scale and/or failed toexploit the unique optical absorption properties of single-layer TMDCs. Here wepresent an experimental realization of a large-area type-II photovoltaicheterojunction using single-layer molybdenum disulfide (MoS2) as the primaryabsorber, by coupling it to the organic {\pi}-donor polymer PTB7. ThisTMDC-polymer heterojunction exhibits photoluminescence intensity that istunable as a function of the thickness of the polymer layer, ultimatelyenabling complete quenching of the TMDC photoluminescence. The strong opticalabsorption in the TMDC-polymer heterojunction produces an internal quantumefficiency exceeding 40% for an overall cell thickness of less than 20 nm,resulting in exceptional current density per absorbing thickness in comparisonto other organic and inorganic solar cells. Furthermore, this work provides newinsight into the recombination processes in type-II TMDC-polymerheterojunctions and thus provides quantitative guidance to ongoing efforts torealize efficient TMDC-based solar cells.

Mutual Photoluminescence Quenching and Photovoltaic Effect in Large-Area Single-Layer MoS2-Polymer Heterojunctions