Codesigning Alloy Compositions of CdSeyTe1−y Absorbers and MgxZn1−xO Contacts to Increase Solar Cell Efficiency.

Thin‐film solar cells such as CdTe are a major commercial photovoltaic technology, with more than 25 GW installed worldwide and levelized costs of electricity competitive with fossil fuels. Further progress may result from integrating CdSeyTe1−y absorbers with MgxZn1−xO contacts, but the device efficiency is difficult to maximize due to coupled dependence on chemical composition of both alloys. Herein, a high‐throughput approach is demonstrated to codesign chemical compositions in alloyed MgxZn1−xO/CdSeyTe1−y thin‐film solar cells, using combinatorial libraries of PV devices with orthogonal composition gradients in CdSeyTe1−y absorbers and MgxZn1−xO contacts. It is found that the solar cell performance is a strong and coupled function of both elemental compositions, with efficiency up to 17.7% (VOC = 836 mV, fill factor = 69%, JSC = 30.6 mA cm−2) at atomic compositions of Mg/(Mg + Zn) ≈18% and average Se/(Se + Te) ≈4%. These performance trends among >100 devices are explained by >100 ns lifetime of photoexcited charge carriers at the MgxZn1−xO/CdSeyTe1−y interface where strong Se accumulation is also observed. This study reports the optimal compositions of the commercially relevant MgxZn1−xO/CdSeyTe1−y solar cells and demonstrates a general approach to codesigning performance of alloyed thin‐film solar cells and other optoelectronic devices. [ABSTRACT FROM AUTHOR]