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Real time energy dispersive X ray diffraction  EDXRD  analysis has been utilized to observe the selenization of Cu Zn Sn S nanoparticle films coated from three nanoparticle populations  Cu  and Sn rich particles roughly 5 nm in size, Zn rich nanoparticles ranging from 10 to 20 nm in diameter, and a mixture of both types of nanoparticles  roughly 1   1 by mass , which corresponds to a synthesis recipe yielding CZTSSe solar cells with reported total area efficiencies as high as 7.9 . The EDXRD studies presented herein show that the formation of copper selenide intermediates during the selenization of mixed particle films can be primarily attributed to the small, Cu  and Sn rich particles. Moreover, the formation of these copper selenide phases represents the first stage of the CZTSSe grain growth mechanism. The large, Zn rich particles subsequently contribute their composition to form micrometer sized CZTSSe grains. These findings enable further development of a previously proposed selenization pathway to account for the roles of interparticle heterogeneities, which in turn provides a valuable guide for future optimization of processes to synthesize high quality CZTSSe absorber layer

The role of interparticle heterogeneities in the selenization pathway of Cu–Zn–Sn–S nanoparticle thin films: a real-time study