We report on order–disorder related band gap changes in Cu2ZnSn(S,Se)4 solar cells which are induced by post-annealing. The band gap changes of the absorber are detected utilizing electroreflectance and analyzed by comparison with predictions of the stochastic Vineyard model. This yields a critical temperature of TC=195 °C above which the Cu2ZnSn(S,Se)4 absorber layer is entirely disordered within the Cu–Zn layers of the kesterite unit cell. The temporal evolution of the band gap during annealing shows that the equilibrium value is reached on a timescale in the order of hours, depending on the annealing temperature. In contrast to other experimental techniques, electroreflectance precisely measures the band gap and is not influenced by defect-mediated radiative recombination.

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In order to identify the impact of the degree of Cu–Zn order in kesterite Cu2ZnSn(S,Se)4 solar cell absorbers on defect states and band tails, we perform photoluminescence (PL), photoluminescence excitation, and time-resolved photoluminescence (TRPL) spectroscopy. The PL lineshape and further PL characteristics such as state filling are analysed as a function of Cu–Zn order. Furthermore, TRPL decays and band tails are quantified. No significant modification in the defect states is caused by changes in Cu–Zn order, meaning that the formation of the defect states is not mainly determined by disorder in the Cu–Zn plane. In regard to band tailing, a small tendency to a decrease in the tailing parameter for the states with a high degree of Cu–Zn order compared to states with a low degree of Cu–Zn order is obvious. However, this reduction is small compared to the reduction of the defect density accompanied by the increase in the degree of Cu–Zn order. Hence, band tails are not mainly formed due to disorder in the Cu–Zn planes.

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