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2D transition metal dichalcogenides (TMDs) are promising candidates for realizing ultrathin and high‐performance photovoltaic devices. However, the external quantum efficiency (EQE) and power conversion efficiency (PCE) of most 2D photovoltaic devices face great challenges in exceeding 50% and 3%, respectively, due to the low efficiency of photocarrier separation and collection. Here, this study demonstrates photovoltaic devices with defect‐free interface and recombination‐free channel based on 2D WS2, showing high EQE of 92% approaching the theoretical limit and high PCE of 5.0%. The high performances are attributed to the van der Waals metal contact without interface defects and Fermi‐level pinning, and the fully depleted channel without photocarrier recombination, leading to intrinsic photocarrier separation and collection with high efficiency. Furthermore, this study demonstrates that the strategy can be extended to other TMDs such as MoSe2 and WSe2 with EQE of 92% and 94%, respectively. This work proposes a universal strategy for building high‐performance 2D photovoltaic devices. The nearly ideal EQE provides great potential for PCE approaching the Shockley–Queisser limit.
A universal strategy for constructing 2D photovoltaic devices with high performances is demonstrated. The device based on 2D WS2 exhibits nearly ideal external quantum efficiency (EQE) of 92% and high power conversion efficiency (PCE) of 5.0%, which are attributed to the defect‐free interface and recombination‐free channel. The nearly ideal EQE provides great potential for PCE approaching the Shockley–Queisser limit.