Predicting magnetic properties and spin relaxation rates in lanthanide-based single-ion magnets

Lanthanide-based single-ion magnets (SIMs) are promising building blocks for the development of new materials with applications in high-density magnetic memory, spintronics, quantum sensing, and quantum computing. These applications require SIMs with stable and controllable magnetic properties, which originate from the electron spin and orbital angular momentum in lanthanide ions. Spin relaxation is responsible for the loss of magnetization in high-density memory applications, while spin decoherence is related to the loss of quantum information in qubits used in quantum sensing and computing. We will describe our theoretical and computational efforts to understand the factors affecting the electron spin relaxation and decoherence in lanthanide complexes and to determine the design criteria for multifunctional lanthanide-based SIMs with useful opto-magnetic properties. The focus will be on the complexes with the terpyridine ligands and different lanthanide ions in the gas, solution, and crystal phases.