Hydrazine solution-processed CuIn(Se,S)2 thin film solar cells: Secondary phases and grain structure

We have carried out microstructural studies of secondary phase formation at the Mo/CuIn(Se,S)2 interface, and of grain structure in hydrazine solution-processed CuIn(Se,S)2 films. The CuIn(Se,S)2 layers were deposited on Mo-coated glasses followed by thermal annealing under a nitrogen ambient. In our previous work, we identified [Cu6S4]2− and [In2(Se,S)4]2− as the two major molecular species present in hydrazine CuIn(Se,S)2 precursor solutions. The CuIn(Se,S)2 films prepared by the precursor solution containing only above two molecular complexes exhibited the undesired secondary interfacial phases such as CuSe and CuIn5S8. It is likely that the reactions between the Mo bottom electrode with sulfur in [Cu6S4]2− can result in the formation of a MoS2 phase, triggering the phase separation of CuIn(Se,S)2 into CuSe and CuIn5S8. To make matters worse, the final CuIn(Se,S)2 films contain a lot of voids that reduce the structural and electrical integrity of the device. The addition of polyselenide molecules [Se]n into the above CuIn(Se,S)2 precursor solutions introduced MoSe2 rather than MoS2 at the back interface which in turn allows sulfur to remain in [Cu6S4]2− complexes. As a result, only the desired phases, CuIn(Se,S)2 and MoSe2, were formed near the back interface. Furthermore, The formation of voids within the film can be also prevented by adding [Se]n into the CuIn(Se,S)2 precursor solution, leading to the formation of a dense film structure.

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► We report microstructural studies for hydrazine solution-processed CuIn(Se,S)2 films.
► [Cu6S4]2− and [In2Se4]2− are essential precursors in forming the CuIn(Se,S)2 phase.
► [Se]n are vital for obtaining desirable microstructure in CuIn(Se,S)2 films.
► Efficiency was improved from 8.9% to 11.1% by adding [Se]n into the precursors.