Intercalated chalcogenides Fe1/4TaS2 and Fe1/3TaS2 under extreme pressure—temperature conditions

Intercalation is an important strategy for enhancing functionality in complex chalcogenides. This is because layered materials can be endowed with intriguing properties by filling the van der Waals gap with various ions and molecules, which, in addition to their unique chemistry, break symmetry in new ways. In order to explore the properties of intercalated metal dichalcogenides under extreme pressure-temperature conditions, we combine diamond anvil cell techniques, Raman scattering spectroscopy, magnetic susceptibility, and first-principles calculations to reveal the pressure–temperature phase diagram of Fe1/3TaS2. This system hosts a compression-driven structural phase transition to a polar state as well as remnant charge density wave signatures deriving from the host lamella of the 2H-parent compound. We also explore the role of different A-site patterns and determine that, by comparison, Fe1/4TaS2 is soft and flexible due to the lower metal density inside the van der Waals gap. These findings open the door to entirely new states of matter with exciting property combinations, including metallicity, polarity, chirality, and altermagnetism – depending upon the conditions – that can support a wide range of spintronics and phononics applications.