Leveraging Surface Siloxide Electronics to Enhance the Relaxation Properties of a Single-Molecule Magnet

Single-molecule magnets (SMMs) hold promise for unmatched information storage density as well applications in quantum computing and spintronics. To date, the most successful SMMs have been organometallic lanthanide complexes. However, their surface immobilization, one of requirements device fabrication commercial application, remains challenging due to sensitivity magnetic properties small changes electronic structure parent SMM. Thus, finding controlled approaches SMM deposition is a timely challenge. In this contribution we apply concept isolobality identify siloxides present at partially dehydroxylated silica suitable replacement archetypal ligand architectures SMMs. We demonstrate theoretically experimentally that isolated siloxide anchoring sites not only enable immobilization but also lead 2 orders magnitude increase magnetization relaxation times.