Publication date: 11th July 2022
Molecular magnetism is an emerging field with potential for technological applications as high-density information storage, quantum computing and spintronics [1]. Molecular systems based on lanthanides are especially promising due to the fundamental properties of lanthanides. Their strong spin-orbit coupling can lead to a high magnetic anisotropy while the strong localization of 4f states reduces the hybridization with surfaces increasing spin lifetimes [2]. Both, a high anisotropy and a large spin lifetime, are essential to increase the magnetic stability and to develop practical applications. Some lanthanide molecular magnet systems have already been reported, as the double-decker phthalocyanine family (LnPc2) [3,4], but up to now the magnetism of lanthanides metal-organic networks remains an unexplored field.
We performed pioneering investigations in this field preparing lanthanide-direct metal-organic networks using three molecular linkers: (i) benzene-1,4-dicarboxylic acid (TPA) coordinated with Dy on Cu(111) [5]; (ii) p-terphenyl-4,4-dicarboxylic acid (TDA) coordinated with Dy and Er on Cu(111) [5]; (iii) 4,4'-Di(4-pyridyl)biphenyl (DPBP) coordinated with Dy and Er on Au(111) [6]. The structural, electronic and magnetic properties were investigated by scanning probe microscopy (STM) and spectroscopy (STS), X-ray linear dichroism (XLD) and X-ray magnetic circular dichroism (XMCD). The experimental results were complemented by density functional theory (DFT) calculations and multiplet calculations. TPA and TDA linkers coordinate with lanthanides in almost square lattices with mononuclear metallic centers, and DPBP forms rhombic binuclear lattices. In both cases the network structure is preserved when the lanthanide atom is exchanged. However, the magnetic properties are drastically altered. The orientation of the easy axis of magnetization and the intensity of the magnetic anisotropy are strongly dependent on the metallic center and the molecular linker. Our results show that it is possible to tailor the magnetic properties of lanthanides by a proper choice of molecular linkers and metallic centers.
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