Metallic transition metal dichalcogenides, such as tantalum diselenide (TaSe2), display quantum correlated phenomena of superconductivity and charge density waves (CDWs) 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 noninvasive and efficient optical methodology detailed here demonstrates an essential link between atomic-scale and microscopic quantum phenomena.