Precise control of multiple spin states on the atomic scale presents a promising avenue for designing and realizing magnetic switches. Despite substantial progress in recent decades, the challenge of achieving control over multiconfigurational reversible switches in low-dimensional nanostructures persists. Our work demonstrates multiple, fully reversible plasmon-driven spin-crossover switches in a single π-d metal-organic chain suspended between two electrodes. The plasmonic nanocavity stimulated by external visible light allows for reversible spin crossover between low- and high-spin states of different cobalt centers within the chain. We show that the distinct spin configurations remain stable for minutes under cryogenic conditions and can be nonperturbatively detected by conductance measurements. This multiconfigurational plasmon-driven spin-crossover demonstration extends the available toolset for designing optoelectrical molecular devices based on SCO compounds.

• Klíčová slova
• density functional theory, light-induced switching, molecular chains, one-dimensional system, scanning tunneling microscopy, spin crossover, transport,
• Publikační typ
• časopisecké články MeSH

The functionality of 2D metal-organic frameworks (MOFs) is crucially dependent on the local environment of the embedded metal atoms. These atomic-scale details are best ascertained on MOFs supported on well-defined surfaces, but the interaction with the support often changes the MOF properties. We elucidate the extent of this effect by comparing the Fe-TCNQ 2D MOF on two weakly interacting supports: graphene and Au(111). We show that the Fe-TCNQ on graphene is nonplanar with iron in quasi-tetrahedral sites, but on Au(111) it is planarized by stronger van der Waals interaction. The differences in physical and electronic structures result in distinct properties of the supported 2D MOFs. The dz2 center position is shifted by 1.4 eV between Fe sites on the two supports, and dramatic differences in chemical reactivity are experimentally identified using a TCNQ probe molecule. These results outline the limitations of common on-surface approaches using metal supports and show that the intrinsic MOF properties can be partially retained on graphene.

• Publikační typ
• časopisecké články MeSH