Realization of long-range magnetic order in surface-supported two-dimensional systems has been challenging, mainly due to the competition between fundamental magnetic interactions as the short-range Kondo effect and spin-stabilizing magnetic exchange interactions. Spin-bearing molecules on conducting substrates represent a rich platform to investigate the interplay of these fundamental magnetic interactions. Here we demonstrate the direct observation of long-range ferrimagnetic order emerging in a two-dimensional supramolecular Kondo lattice. The lattice consists of paramagnetic hexadeca-fluorinated iron phthalocyanine (FeFPc) and manganese phthalocyanine (MnPc) molecules co-assembled into a checkerboard pattern on single-crystalline Au(111) substrates. Remarkably, the remanent magnetic moments are oriented in the out-of-plane direction with significant contribution from orbital moments. First-principles calculations reveal that the FeFPc-MnPc antiferromagnetic nearest-neighbour coupling is mediated by the Ruderman–Kittel–Kasuya–Yosida exchange interaction via the Au substrate electronic states. Our findings suggest the use of molecular frameworks to engineer novel low-dimensional magnetically ordered materials and their application in molecular quantum devices.

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Background:Inorganic resists show promising performances in extreme ultraviolet (EUV) lithography. Yet, there is a need for understanding the exact chemical mechanisms induced by EUV light on these materials. Aim:To gain knowledge on the EUV chemistry of inorganic resists, we investigate hybrid inorganic–organic molecular compounds, metal oxoclusters (MOCs). Their molecular nature allows for the monitoring of specific structural changes by means of spectroscopy and thus for the elucidation of the mechanisms behind pattern formation. Approach:We compare the sensitivity of MOCs based on Zr and Hf, and methacrylate ligands as EUV resists. The chemical and structural changes causing the solubility switch were investigated by ex situ x-ray spectroscopy, infrared spectroscopy, ultraviolet–visible spectroscopy, and grazing incidence x-ray scattering. Results:Higher sensitivity was detected for the Hf-based material, in line with its higher absorptivity. A small fraction of the carboxylate ligands is lost at doses that yield solubility contrast, whereas aggregation of the inorganic clusters was not observed. Conclusions:These results provide evidence that, although the mechanism of solubility switch in these materials starts with decarboxylation reactions, it mainly proceeds through cross linking of the organic shells instead of aggregation of the inorganic clusters.