Pressure-induced superconductivity and isosymmetric structural transition in quasi-one-dimensional Ta2PdS6

Quasi-one-dimensional materials are a promising system for future applications in electronics and optoelectronics. The refinement of the strong interaction mechanism in quasi-one-dimensional crystals under extreme conditions is still challenging. Here we report a thorough study of superconductivity and phase transition in pressurized Ta₂PdS₆ by electrical transport, in situ x-ray diffraction (XRD), Raman spectroscopy, and density functional calculation. Ta₂PdS₆ experiences valence bands crossing the Fermi level to form a set of small hole pockets at P3. 7 GPa, which drives the system from a semiconductor to a metal. The pressure-induced superconductivity occurs with decreasing temperature, accompanied by a monoclinic distortion at the critical pressure P₂30. 8 GPa. Both XRD measurements and theoretical calculations provide evidence that this structural transition is determined to be isosymmetric, mainly resulting from rearrangement of the S atoms along the a and c axes, indicative of the importance of electron-lattice coupling. When the pressure increases to 82 GPa, the high pressure phase has a very high density of electron states at the Fermi level with T₂^onset4pt{0ex} 5. 2 K, likely mediated by strongly electron-coupled phonons. The present study proposes an alternative approach to investigate the effects of pressure on crystal distortion and superconductivity.