The stability of magnetic information stored in surface adsorbed single-molecule magnets is of critical interest for applications in nanoscale data storage or quantum computing. The present study combines X-ray magnetic circular dichroism, density functional theory and magnetization dynamics calculations to gain deep insight into the substrate dependent relevant magnetization relaxation mechanisms. X-ray magnetic circular dichroism reveals the opening of a butterfly-shaped magnetic hysteresis of DyPc2 molecules on magnesium oxide and a closed loop on the bare silver substrate, while density functional theory shows that the molecules are only weakly adsorbed in both cases of magnesium oxide and silver. The enhanced magnetic stability of DyPc2 on the oxide film, in conjunction with previous experiments on the TbPc2 analogue, points to a general validity of the magnesium oxide induced stabilization effect. Magnetization dynamics calculations reveal that the enhanced magnetic stability of DyPc2 and TbPc2 on the oxide film is due to the suppression of two-phonon Raman relaxation processes. The results suggest that substrates with low phonon density of states are beneficial for the design of spintronics devices based on single-molecule magnets.

Center for Quantum Nanoscience Institute for Basic Science 03760 Seoul Republic of Korea

Centre National de la Recherche Scientifique Paris Sciences et Lettres Sorbonne Université F 75005 Paris France

Département de Chimie École Normale Supérieure F 75005 Paris France

Department of Physics Ewha Womans University 03760 Seoul Republic of Korea

Institut de Physique et Chimie des Matériaux de Strasbourg Université de Strasbourg 23 rue du Loess BP 43 F 67034 Strasbourg Cedex 2 France

Institute of Nanotechnology Hermann von Helmholtz Platz 1 D 76344 Eggenstein Leopoldshafen Germany

Institute of Physics Station 3 CH 1015 Lausanne Switzerland

Institute of Physics The Czech Academy of Sciences Cukrovarnická 10 CZ 162 00 Prague 6 Czech Republic

Swiss Light Source Paul Scherrer Institut CH 5232 Villigen Switzerland

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On-Surface Synthesis of Organolanthanide Sandwich Complexes

Lanthanide metal-organic network featuring strong perpendicular magnetic anisotropy