Co-Designing Alloy Compositions of CdSeyTe1-y Absorbers and MgxZn1-xO Contacts to Increase Solar Cell Efficiency: Article No. 2200394

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 CdSe_yTe_1−y absorbers with Mg_xZn_1−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 Mg_xZn_1−xO/CdSe_yTe_1−y thin-film solar cells, using combinatorial libraries of PV devices with orthogonal composition gradients in CdSe_yTe_1−y absorbers and Mg_xZn_1−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% (V_OC = 836 mV, fill factor = 69%, J_SC = 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 Mg_xZn_1−xO/CdSe_yTe_1−y interface where strong Se accumulation is also observed. This study reports the optimal compositions of the commercially relevant Mg_xZn_1−xO/CdSe_yTe_1−y solar cells and demonstrates a general approach to codesigning performance of alloyed thin-film solar cells and other optoelectronic devices.