Self-organization process of framboidal pyrite investigated by microtextural analysis

The 3D packing structures of microcrystals in framboidal pyrite have been investigated by morphological observations and crystallographic orientation analyses using the EBSD technique to understand its self-organization process. The packing structures are basically classified into three types: (i) face-centered cubic (fcc), (ii) icosahedral and (iii) random packings. The orientation analyses on many ordered (fcc) framboids revealed that about a half of the microcrystals in a framboid involve high-angle (~ 90°) misorientation. This means that even in morphologically highly ordered framboids, the crystallographic orientations of microcrystals are not uniform, suggesting that the self-organization process of framboidal microcrystals is not crystallographically controlled. We propose a three-step model for the self-organization: (1) simultaneous nucleation of monodispersive pyrite microcrystals in a fixed volume (from precursor FeS), (2) aggregation of the randomly oriented microcrystals driven by surface forces and the reduction in total surface energy associated with both the individual microcrystals and the whole aggregate, resulting in the formation of the framboidal texture, and 3) reorientation of the microcrystals driven by further reduction in surface energy associated with the grain boundaries.