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This joint experimental and theoretical study of the structural, vibrationaland electrical properties of rhombohedral SnSb2Te4 at high pressure unveils theinternal mechanisms of its compression. The equation of state and the internalpolyhedral compressibility, the symmetry and behavior of the Raman-active modesand the electrical behavior of this topological insulator under compressionhave been discussed and compared with the parent binary alpha-Sb2Te3 and SnTecompounds and with related ternary compounds. Our X-ray diffraction and Ramanmeasurements together with theoretical calculations, which include topologicalelectron density and electronic localization function analysis, evidence thepresence of an isostructural phase transition around 2 GPa and a Fermiresonance around 3.5 GPa. The Raman spectrum of SnSb2Te4 shows vibrationalmodes that are forbidden in rocksalt SnTe; thus showing a novel way toexperimentally observe the forbidden vibrational modes of some compounds.Additionally, since SnSb2Te4 is an incipient metal, like its parent binarycompounds, we establish a new criterion to identify the recently proposedmetavalent bonding in complex materials when different bond characters coexistin the system. Finally, SnSb2Te4 exhibits a pressure-induced decomposition intothe high-pressure phases of its parent binary compounds above 7 GPa, which issupported by an analysis of their formation enthalpies. We have framed thebehavior of SnSb2Te4 within the extended orbital radii map of BA2Te4 compounds,which paves the way to understand the pressure behavior and stability ranges ofother layered van der Waals-type compounds with similar stoichiometry.

Characterization and decomposition of the natural van der Waals heterostructure SnSb2Te4 under compression