Tunable Mirror‐Symmetric Type‐III Ising Superconductivity in Atomically‐Thin Natural Van der Waals Heterostructures

Van der Waals (vdW) crystals with strong spin-orbit coupling (SOC) provide great opportunities for exploring unconventional 2D superconductors, wherein new pairing states emerge due to the interplay of SOC with crystalline symmetries, electronic correlations, quenched disorders and external modulation forces, etc. Here, a distinct mirror-symmetry protected Ising pairing state with unprecedented Γ- and M-valley symmetries in natural vdW heterostructures (vdWH) of interweaving tetragonal SnSe and trigonal 1H-TaSe₂ monolayers is reported, in which the unidirectional lattice interlocking effectively suppresses the K-valley Ising pairing mechanism by incommensurate charge-density-wave (CDW) transitions. In the 2D limit of an TaSe₂/SnSe bilayer with intact basal mirror symmetry (M_z), the mirror-symmetric vdWH Ising superconductors show anomalous in-plane magnetic field B_‖-controlled enhancements in the critical temperature T_c, which is completely absent for multilayer vdWHs with broken M_z induced by orthorhombic stacking between nearest-neighbour TaSe₂ monolayers. The experimental observations consistently reveal a mirror symmetry-protected type-III Ising state in the inversion asymmetric lattice of 1H-TaSe₂, which is predicted to be a mixture of spin-singlet and spin-triplet states.