Quantifying Quasi‐Fermi Level Splitting and Mapping its Heterogeneity in Atomically Thin Transition Metal Dichalcogenides

One of the most fundamental parameters of any photovoltaic material is its quasi‐Fermi level splitting (?µ) under illumination. This quantity represents the maximum open‐circuit voltage (V_oc) that a solar cell fabricated from that material can achieve. Herein, a contactless, nondestructive method to quantify this parameter for atomically thin 2D transition metal dichalcogenides (TMDs) is reported. The technique is applied to quantify the upper limits of V_oc that can possibly be achieved from monolayer WS₂, MoS₂, WSe₂, and MoSe₂‐based solar cells, and they are compared with state‐of‐the‐art perovskites. These results show that V_oc values of ≈1.4, ≈1.12, ≈1.06, and ≈0.93 V can be potentially achieved from solar cells fabricated from WS₂, MoS₂, WSe₂, and MoSe₂ monolayers at 1 Sun illumination, respectively. It is also observed that ?µ is inhomogeneous across different regions of these monolayers. Moreover, it is attempted to engineer the observed ?µ heterogeneity by electrically gating the TMD monolayers in a metal‐oxide‐semiconductor structure that effectively changes the doping level of the monolayers electrostatically and improves their ?µ heterogeneity. The values of ?µ determined from this work reveal the potential of atomically thin TMDs for high‐voltage, ultralight, flexible, and eye‐transparent future solar cells.