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Probing NaCl hydrate formation from aqueous solutions by Terahertz Time-Domain SpectroscopyThe cooling-induced formation of hydrate in aqueous NaCl solutions was probed using terahertz time-domain spectroscopy (THz-TDS). It was found that the NaCl hydrate formation is accompanied with emergence of four new absorption peaks at 1.60, 2.43, 3.34 and 3.78 THz. Combining the X-ray diffraction measurement with the solid-state based density functional theory (DFT) calculations, we assign the observed terahertz absorption peaks to the vibrational modes of the formed NaCl⋅2H2O hydrate during cooling. This work dedicates THz-TDS based analysis great potential in studying ionic hydrate and the newly revealed collective vibrational modes could be the sensitive indicators to achieve quantitative analysis in phase transitions and lattice dynamics.