Abstract: | Different techniques were used to follow the transformation of CdS platelets during grinding and under hydrostatic pressure. X‐ray diffraction and transmission electron microscopy revealed that the platelets included zinc blende (cubic) CdS nanodomains dispersed in a wurtzite (hexagonal) single‐crystalline matrix. Extended grinding led to a decrease of the grain size and to a progressive transformation of the hexagonal stacking into a cubic one. The same phase transition was observed up to 9 GPa under hydrostatic pressure. Off‐resonance Raman spectra collected at different stages of the transition led us to connect band groups that were usually overlooked (in resonance conditions) or considered separately. They all probe the stacking disorder and their intensity can be related to the density of stacking faults. Off‐resonance Raman spectroscopy offers a way of probing the optical properties of CdS (and, more generally, layered semiconductors) as a function of the structure and of the confinement of vibrations by structural defects. Copyright © 2011 John Wiley & Sons, Ltd. |