Controlled Modification of Superconductivity in Epitaxial Atomic Layer-Organic Molecule Heterostructures

Self-assembled organic molecules can potentially be an excellent source of charge and spin for two-dimensional (2D) atomic-layer superconductors. Here we investigate 2D heterostructures based on In atomic layers epitaxially grown on Si and highly ordered metal-phthalocyanine (MPc, M = Mn, Cu) through a variety of techniques: scanning tunneling microscopy, electron transport measurements, angle-resolved photoemission spectroscopy, X-ray magnetic circular dichroism, and ab initio calculations. We demonstrate that the superconducting transition temperature (Tc) of the heterostructures can be modified in a controllable manner. Particularly, the substitution of the coordinated metal atoms from Mn to Cu is found to reverse the Tc shift from negative to positive directions. This distinctive behavior is attributed to a competition of charge and spin effects, the latter of which is governed by the directionality of the relevant d-orbitals. The present study shows the effectiveness of molecule-induced surface dopin...