Abstract
Interfaces are critical in quantum physics, and therefore we must explore the potential for designer hybrid materials that profit from promising combinatory effects. In particular, the fine-tuning of spin polarization at metallo–organic interfaces opens a realm of possibilities, from the direct applications in molecular spintronics and thin-film magnetism to biomedical imaging or quantum computing. This interaction at the surface can control the spin polarization in magnetic field sensors, generate magnetization spin-filtering effects in nonmagnetic electrodes, or even give rise to a spontaneous spin ordering in nonmagnetic elements such as diamagnetic copper and paramagnetic manganese.
Charge transfer at metallo–molecular interfaces may be used to design multifunctional hybrids with an emergent magnetization that may offer an eco-friendly and tunable alternative to conventional magnets and devices. Here, we investigate the origin of the magnetism arising at these interfaces by using different techniques to probe 3d and 5d metal films such as Sc, Mn, Cu, and Pt in contact with fullerenes and rf-sputtered carbon layers. These systems exhibit small anisotropy and coercivity together with a high Curie point. Low-energy muon spin spectroscopy in Cu and Sc–C
60
multilayers show a quick spin depolarization and oscillations attributed to nonuniform local magnetic fields close to the metallo–carbon interface. The hybridization state of the carbon layers plays a crucial role, and we observe an increased magnetization as sp
3
orbitals are annealed into sp
2
−π graphitic states in sputtered carbon/copper multilayers. X-ray magnetic circular dichroism (XMCD) measurements at the carbon K edge of C
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layers in contact with Sc films show spin polarization in the lowest unoccupied molecular orbital (LUMO) and higher π*-molecular levels, whereas the dichroism in the σ*-resonances is small or nonexistent. These results support the idea of an interaction mediated via charge transfer from the metal and
dz
–π hybridization. Thin-film carbon-based magnets may allow for the manipulation of spin ordering at metallic surfaces using electrooptical signals, with potential applications in computing, sensors, and other multifunctional magnetic devices.