With their intrinsic slow relaxation of magnetization in the absence of the applied field single-molecule magnets (SMMs) hold great promise for quantum information science applications. Engendering such magnetic properties requires the right combination of paramagnetic metal center(s) and precisely tailored ligand environment. Over the years a wealth of work has been devoted to understanding the design principles for high-performing SMMs. This has led to identification of organolanthanide complexes featuring substituted cyclopentadienyl ligands as the best-performing systems to date. While improvement of the intrinsic magnetic properties of these molecules is important, future practical implementation in devices requires strategies for their surface deposition. This constitutes a great challenge as interaction with surface alters the delicate electronic structure and geometry of the parent complex and often leads to loss of the SMM properties.<br/>In this talk I will describe a novel concept in surface immobilization of SMMs that leverages the principles of surface organometallic chemistry (SOMC). Using a well-established organometallic SMM as a test system I will demonstrate that surface deposition by SOMC not only preserves the parent complex’s hysteretic behavior, but also yields improvement of the magnetic relaxation characteristics by two orders of magnitude. This is only possible by rational choice of the supporting material, partially dehydroxylated silica in this case, that can act as a surrogate for the classical ligand architectures used in the design of state-of-the-art SMMs, and thus mimic the coordination environment present in the parent species.

Improvement of single-molecule magnet performance via the surface organometallic chemistry approach

ACS Spring Meeting 2021

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