Vibrational properties and ultrafast photocarrier dynamics of 2H–TaS2 under pressures are studied by the experiments of Raman scattering and femtosecond time resolved spectroscopy. With increasing pressure, the linewidth of two-phonon Raman mode broadens, especially features with a sudden rapid increase above 10 GPa. Meanwhile, the ultrafast dynamics show that the fast decay through optical phonon scattering is significantly suppressed in amplitude and prolonged in lifetime; however, the weight of the slow decay component originating from acoustic phonon scattering is enhanced at high pressures. Furthermore, the electron-phonon (e-ph) coupling constant, λq, and the density of states (DOS) near the Fermi level, N(0), are evaluated qualitatively, which reveals a drastic decrease in e-ph coupling strength and a sudden increase in the DOS beyond 10 GPa. This turning pressure is consistent with the critical point where Tc of superconductivity peaks while the charge density wave (CDW) vanishes, indicating the direct correlations between λq, N(0), superconductivity, and the CDW under pressure. The anomaly of the DOS may imply the occurrence of a topological transition of the electronic structure. Our work not only provides valuable information for the understanding of competition between the CDW and superconductivity in 2H–TaS2 but also may open up a routine to unveil the pressure-induced electronic topological transition.

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