Tuning quantum paramagnetism and d-wave superconductivity in single-layer iron chalcogenides by chemical pressure

By substituting S into single-layer FeSe/SrTiO3, chemical pressure is applied to tune its paramagnetic state that is modeled as an incoherent superposition of spin-spiral states. The resulting electronic bands resemble an ordered checkerboard antiferromagnetic structure, consistent with angle-resolved photoemission spectroscopy measurements. Scanning tunneling spectroscopy reveals a gap evolving from U-shaped for FeSe to V-shaped for FeS with decreasing size, attributed to a d-wave superconducting state for which nodes emerge once the gap size is smaller than the effective spin-orbit coupling.