Superhigh Uniform Magnetic Cr Substitution in a 2D Mo2C Superconductor for a Macroscopic-Scale Kondo Effect

Substitutional doping provides an effective strategy to tailor the properties of 2D materials, but it remains an open challenge to achieve tunable uniform doping, especially at high doping level. Here, uniform lattice substitution of a 2D Mo2C superconductor by magnetic Cr atoms with controlled concentration up to approximate to 46.9 at% by chemical vapor deposition and a specifically designed Cu/Cr/Mo trilayer growth substrate is reported. The concentration of Cr atoms can be easily tuned by simply changing the thickness of the Cr layer, and the samples retain the original structure of 2D Mo2C even at a very high Cr concentration. The controlled uniform Cr doping enables the tuning of the competition of the 2D superconductor and the Kondo effect across the whole sample. Transport measurements show that with increasing Cr concentration, the superconductivity of the 2D Cr-doped Mo2C crystals disappears along with the emergence of the Kondo effect, and the Kondo temperature increases monotonously. Using scanning tunneling microscopy/spectroscopy, the mechanism of the doping level effect on the interplay and evolution between superconductivity and the Kondo effect is revealed. This work paves a new way for the synthesis of 2D materials with widely tunable doping levels, and provides new understandings on the interplay between superconductivity and magnetism in the 2D limit.