12.3% Efficient Low V_oc Loss Pure Sulfide Kesterite Solar Cells from DMSO Solution via Cadmium Alloying

Abstract

Cd alloying has been theoretically proved to be an effective strategy to suppress Cu‐Zn antisite defects and related defect cluster for improving device performance of pure sulfide kesterite Cu₂ZnSnS₄ (CZTS) thin film solar cells. However, the potential of Cd alloying has not been fully realized by solely doping without further post heat‐treatment. Here, Cd alloying CZTS (Cu₂(Zn,Cd)SnS₄, CZCTS) is reported through dimethyl sulfoxide (DMSO) solution and how alloying concentration affects reaction path, grain growth, and electronic properties of the CZCTS absorbers is investigated. This study found that Cd can be incorporated into CZTS through direct phase transformation grain growth, which sufficiently suppresses band tailing. High quality CZCTS absorber films and efficient solar cells are fabricated within a wide range of alloy concentration. A champion CZCTS device with a power conversion efficiency of 12.3% is achieved at 35% Cd concentration without any post heat treatment, improved by over 70% compared to 7.0% of CZTS. This device exhibits a high V_OC gain to the Shockley–Queisser (Voc/Voc^SQ = 59.7%), the lowest V_OC deficit achieved in pure sulfide kesterite solar cells. The results demonstrate the importance of the Cd alloying strategy for mitigating band tailing and achieving high efficiency pure sulfide kesterite solar cells.