The Se content in
a Cu2ZnSn(S, Se)4 absorber layer has a significant
impact on the electronic properties, but it is rather challenging
to control the Se/(S + Se) ratio due to a complicated selenization
process. Here, a low-toxicity thiol/amine-based solution process was
developed to tune the Se content in a Cu2ZnSn(S, Se)4 absorber layer to an optimal value by ingeniously controlling
the SeO2 in the precursor solution. We demonstrated that
the crystal growth and the band gap of Cu2ZnSn(S, Se)4 thin films are affected by the Se/(S + Se) ratio. By this
approach, the open-circuit voltage deficit (V
oc,def) of the device was effectively decreased, and the short-circuit
density (J
sc) and fill factor (FF) were
remarkably improved; thus, the power conversion efficiency of the
Cu2ZnSn(S, Se)4 solar cells was successfully
increased from 5.6% to 9.7% for the optimal band gap (E
g = 1.13 eV).