Evolution of cation ordering and crystal defects controlled by Zn substitutions in Cu2SnS3 ceramics

Chao Li, Haili Song, Yawei Shen, Yifeng Wang, Yan Cheng, Ruijuan Qi, Shiyou Chen, Chungang Duan, Rong Huang

Research output: Contribution to journalArticlepeer-review

6 Scopus citations

Abstract

The microstructures of a series of Cu2ZnxSn1-xS3 (x = 0, 0.05, 0.10, 0.15,0.20) ceramic samples are investigated by a combination of selected area electron diffraction (SAED), high-resolution transmission electron microscopy (HRTEM), high-angle annular dark-field imaging (HAADF) and X-ray energy dispersive spectroscopy (EDS) techniques. The pure Cu2SnS3 sample takes the monoclinic structure with the ordering of eight 3Cu-Sn and four 2Cu-2Sn clusters, which obey the octet rule. With the increase of Zn substitution, unique mosaic-type nanostructures comprising well-defined cation-disordered domains coherently bonded to a surrounding network phase with semi-ordered cations are formed in the matrix grains. The atomic structures of the semi-ordered phases are revealed as CuInS2-like phase (Zn < 5 atom%), Cu6ZnSn3S10 (Cu2SnS3: ZnS = 3:1) and Cu4ZnSn2S7 (Cu2SnS3: ZnS = 2:1), respectively. These ordered structures derive from the zinc blende structure (201) superlattice of -(Cu-S)2(Zn-S)(Sn-S)- in the kesterite Cu2ZnSnS4 (Cu2SnS3:ZnS = 1:1). Meanwhile, point defects, dislocations, stacking faults, and finally Cu2-xS nanoprecipitates are formed sequentially to compromise the excessive Cu ions when the Zn contents increase from 5 atom% to 20 atom%. Understanding of the concurrence and evolution of the cation ordering and crystal defects are important to tailor their microstructures and physical properties in the Cu-Zn-Sn-S quaternary system.

Original languageEnglish
Article number105322
JournalAIP Advances
Volume8
Issue number10
DOIs
StatePublished - 1 Oct 2018

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