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This study represents the investigation of earth-abundant and non-toxic CZTSSe absorber materials in kesterite solar cell by using the Finite Element Method (FEM) with (1) electrical, and (2) optical approaches. The simulated results have been validated with the experimental results to define guidelines for boosting the cell performance. For improving the cell efficiency, potential barrier variations in the front contact, and the effect of different lattice defects in the CZTSSe absorber layer have been examined. Controlling the defects and the secondary phases of absorber layer have significant influence on the cell performance improvement. Previous studies have demonstrated that, synthesis of CZTSSe:Na nanocrystals and controlling the S/(S + Se), Cu/(Zn + Sn), and Zn/Sn ratios (stoichiometry) have significant effects on the reduction of trap-assisted recombination (Shockley–Read–Hall recombination model). In this work, a screening-based approach has been employed to study the cell efficiency over a wide range of defect densities. Two categorized defect types including benign defects ($${N}_{t}<{10}^{16}$$ N t < 10 16 cm−3 , Nt defines trap density) and harmful defects $${(N}_{t}>{10}^{16}$$ ( N t > 10 16 cm−3) in the absorber bandgap in the CZTSSe solar cell, by analyzing their position changes with respect to the electron Fermi level (Efn) and the Valence Band Maximum positions have been identified. It is realized that, the harmful defects are the dominant reason for the low efficiency of the kesterite solar cells, therefore, reducing the number of harmful defects and also total defect densities lead to the power conversion efficiency record of 19.06%. This increment makes the CZTSSe solar cells as a promising candidate for industrial and commercial applications.

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