Phonon origin and lattice evolution in charge density wave states

Abstract

Metallic transition metal dichalcogenides, such as tantalum diselenide (TaSe2), display quantum correlated phenomena of superconductivity and charge density waves (CDW) at low temperatures. Here, the photophysics of 2H-TaSe₂ during CDW transitions is revealed by combining temperature-dependent, low-frequency Raman spectroscopy and density functional theory (DFT). The spectra contain amplitude, phase, and zone-folded modes that are assigned to specific phonons and lattice restructuring predicted by DFT calculations with superb agreement. The non-invasive and efficient optical methodology detailed here demonstrates an essential link between atomic-scale and microscopic quantum phenomena.