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-TaSe(2) 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.