The optimal fraction of Mg incorporation in sputter‐deposited MgXZn1−XO (MZO) emitters for thin‐film CdTe‐based solar cells is evaluated by varying it over a range of x from 0 to 0.35. This range allows a variation in the conduction band offset from −0.1 eV (cliff like) to +0.32 eV (spike like). A maximum efficiency of 18.5% for cells with the bilayer CdSeTe/CdTe absorber occurs at x = 0.15, which corresponds to a spike‐like band offset near 0.2 eV, as confirmed by X‐ray photoelectron spectroscopy. In addition, good cell performance is seen over a fairly broad range of x extending from 0.1 to 0.25. The MZO optical bandgap increases with the Mg fraction, consistent with an increasing conduction band offset. Temperature‐dependent current−voltage measurements and time‐resolved photoluminescence show improvement in the emitter/absorber interface with the incorporation of Mg. Capacitance−voltage measurements show that the depletion region extends further into the absorber with more Mg, and X‐ray diffraction confirms a change from a hexagonal‐dominant crystal structure toward zinc blende at x = 0.35.
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