Record‐High Superconductivity in Transition Metal Dichalcogenides Emerged in Compressed 2H‐TaS₂

Abstract Pressure has always been an effective method for uncovering novel phenomena and properties in condensed matter physics. Here, an electrical transport study is carried on 2H‐TaS₂ up to ≈208 GPa, and an unexpected superconducting state (SC‐II) emerging around 86.1 GPa with an initial critical temperature (T_c) of 9.6 K is found. As pressure increases, the T_c enhances rapidly and reaches a maximum of 16.4 K at 157.4 GPa, which sets a new record for transition metal dichalcogenides (TMDs). The original superconducting state (SC‐I) is found to be re‐enhanced above 100 GPa after the recession around 10 GPa, and coexists with SC‐II to the highest pressure applied in this work. In situ high‐pressure X‐ray diffraction and Hall effect measurements reveal that the occurrence of SC‐II is accompanied by a structural modification and a concurrent enhancement of hole carrier density. The new high‐T_c superconducting state in 2H‐TaS₂ can be attributed to the change of the electronic states near the Fermi surface, owing to pressure‐induced interlayer modulation. It is the first time finding this remarkable superconducting state in TMDs, which not only brings a new broad of perspective on layered materials but also expands the field of pressure‐modified superconductivity.