Executive Summary : | Single-molecule magnets (SMMs) are compounds that exhibit slow magnetization even after removing the magnetic field and exhibit molecular hysteresis. They have been explored in high-density information storage devices, quantum computing, and molecular spintronics. The most significant achievement in this area is the observation of the magnetization blockade up to 80 K for organometallic sandwiched type [DyCp2]+ complexes. However, to use these SMMs, the magnetization blockade barrier must be raised above room temperature, which is challenging due to fast quantum tunnelling of magnetization and spin-phonon relaxation processes. Additionally, end-user applications require sufficient resilience upon grafting in two- and three-dimensional architectures to access individual molecules as magnetic bits for read-and-write processes.
This proposal aims to address these challenges by computational modeling of the magnetic properties of SMMs and SMMs grafted on surfaces and 3D networks. High-level CASSCF/PT2 and MC-PDFT calculations will be performed to compute the magnetic properties of the Ln(III) based SMM and the magnetic relaxation rate in a more realistic crystal lattice environment. New design criteria will be proposed to increase the magnetic blockade barrier of Ln(III) based SMMs. The proposal also aims to model SMMs in metal-organic frameworks (MOFs) to study their structural, electronic, and magnetic properties. |