Superconductivity is mutually exclusive with ferromagnetism, because the ferromagnetic exchange field is often destructive to superconducting pairing correlation. Well-designed chemical and physical methods have been devoted to realize their coexistence only by structural integrity of inherent superconducting and ferromagnetic ingredients. However, such coexistence in freestanding structure with nonsuperconducting and nonferromagnetic components still remains a great challenge up to now. Here, we demonstrate a molecule-confined engineering in two-dimensional organic-inorganic superlattice using a chemical building-block approach, successfully realizing first freestanding coexistence of superconductivity and ferromagnetism originated from electronic interactions of nonsuperconducting and nonferromagnetic building blocks. We unravel totally different electronic behavior of molecules depending on spatial confinement: flatly lying Co(Cp) molecules in strongly confined SnSe interlayers weaken the coordination field, leading to spin transition to form ferromagnetism; meanwhile, electron transfer from cyclopentadienyls to the Se-Sn-Se lattice induces superconducting state. This entirely new class of coexisting superconductivity and ferromagnetism generates a unique correlated state of Kondo effect between the molecular ferromagnetic layers and inorganic superconducting layers. We anticipate that confined molecular chemistry provides a newly powerful tool to trigger exotic chemical and physical properties in two-dimensional matrixes.
Correlated electronic materials (CEMs) with strong electron−electron interactions are often associated with exotic properties, such as metal‐insulator transition (MIT), charge density wave (CDW), superconductivity, and magnetoresistance (MR), which are fundamental to next generation condensed matter research and electronic devices. When the dimension of CEMs decreases, exposing extremely high specific surface area and enhancing electronic correlation, the surface states are equally important to the bulk phase. Therefore, surface/interface chemical interactions provide an alternative route to regulate the intrinsic properties of low‐dimensional CEMs. Here, recent achievements in surface/interface chemistry engineering of low‐dimensional CEMs are reviewed, using surface modification, molecule−solid interaction, and interface electronic coupling, toward modulation of conducting solids, phase transitions including MIT, CDW, superconductivity, and magnetism transition, as well as external‐field response. Surface/interface chemistry engineering provides a promising strategy for exploring novel properties and functional applications in low‐dimensional CEMs. Finally, the current challenge and outlook of the surface/interface engineering are also pointed out for future research development.
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