The role of secondary phase precipitation on grain boundary electrical activity in Cu2ZnSnS4 (CZTS) photovoltaic absorber layer material

Abstract

Cathodoluminescence is used to measure the recombination velocity of the heterointerfaces between Cu2ZnSnS4 (CZTS) and CuxSnySz, SnS secondary phases precipitated along the grain boundaries as well as ZnS precipitated within the CZTS grain interiors. The CZTS/CuxSnySz and CZTS/ZnS heterointerfaces had recombination velocities smaller than the bulk carrier diffusion velocity while the opposite is true for the CZTS/SnS heterointerface. Secondary phases having crystal structures compatible with CZTS (e.g., ZnS, Cu2SnS3) are likely to form heterointerfaces with small misfit strain and hence low interfacial recombination velocity. The precipitation of such secondary phases along grain boundaries in CZTS provides a novel mechanism for grain boundary passivation. However, it is not known if grain boundary passivating secondary phases would necessarily increase the overall photovoltaic device efficiency since other factors, such as the band gap of the secondary phase compared to the Shockley-Queisser ideal value and the nature of the heterointerface between CZTS (i.e., type-I vs type-II), also affect device operation and must therefore be taken into consideration.