A DFT Study of Structure, Electronic and Optical Properties of Se-Doped Kesterite Cu2ZnSnS4 (CZTSSe)

In this work, we have studied the geometric structure and electronic and optical properties of Cu2ZnSn(S1-xSex)4 nanocrystals where x = 0, 0.25, 0.50, 0.75, 1.00 by the quantum-chemical calculations within the framework of DFT. For the electronic and optical properties calculations, the effective XC functional and the TB-mBJ potential were used. The calculated structural characteristics show that the volume of these systems increases with increasing the Se concentration. The electronic properties of the Se-doped kesterite Cu2ZnSnS4 show that the bandgap tends to decrease. It was found that the Se-doped material has noticeably increased its absorption capacity. Hence, the efficiency of the Cu2ZnSnS4 in the IR region of radiation improves. The effective reduction bandgap from 1.455 eV to 0.94 eV is observed, which is in gоod agreement with known experimental data for the pure and undoped systems Cu2ZnSnS4 and Cu2ZnSnSе4. The calculated band gap is 1.346 eV for the Cu2ZnSnS3Se system, which is comparable with the optimal bandgap of semiconductors used in photovoltaic applications. It was found that with the increase of the Se concentration, the absorption coefficient increases, thereby resulting in the materials' reflectivity decrease. The calculated optoelectronic parameters and the density of electronic states indicate that the Cu2ZnSnS4:Se system possesses a favorable property, suitable for applications in solar cells technology.