Improving the charge separation and collection at the buffer/absorber interface by double-layered Mn-substituted CZTS

A non-ideal buffer-absorber interface due to interface recombination is one of the limitations in Cu2ZnSnS4 (CZTS) solar cells. An absorber gradient using partial cation-substitution is one possible solution to this issue by reducing interface recombination sites and improving band alignment. Partial substitution of Zn with Mn is a potentially attractive concept owing to its abundance as well as similar size and electronic properties compared to Zn. In this study, Cu2MnxZn1-xSnS4 (CMZTS) thin film were fabricated by a sol-gel spin coating technique to understand the effect of Mn on the device performance. X-ray diffraction (XRD) and Raman analysis confirm Mn substitution for Zn in the crystal lattice of Cu2ZnSnS4 (CZTS) with no secondary phases detected for x ≤ 0.4. Enhancement of short circuit current (Jsc) in Cu2Mn0.15Zn0.85SnS4 has led to improved efficiency in comparison with CZTS. Since external quantum efficiency (EQE) indicates the short wavelength collection as the main reason for the improved Jsc, we designed a double layered structure of CZTS as bottom layer and CM0.15Z0.85TS as top layer. With this structure, we obtained our best performance cell with power conversion efficiency (PCE) of 5.73% and Jsc of 17.86 mA/cm2. The improved Jsc is attributed to increased depletion width and higher activation energy of the limiting recombination mechanism as shown by capacitance-voltage and temperature dependent current-voltage measurements. Our study concludes that CM0.15Z0.85TS top layer improves the interface quality of the p-n junction and may be an alternative method to improve the performance of CZTS solar cells.