Molecular magnetism has emerged as a fertile ground for uncovering new regimes of spin dynamics and electronic ordering, where chemical control translates directly into magnetic functionality [1].Three prototypical classes illustrate this diversity. Spin crossover (SCO) complexes exhibit bistable spin-state transitions driven by external stimuli, with collective ordering and cooperative elastic interactions giving rise to hysteresis, memory effects, and slow relaxation across energy barriers [2-3]. Valence tautomeric (VT) systems show electron transfer between metal and ligand sites, often situated at the Robin-Day II/III boundary, where intervalence charge transfer and electron hopping generate dynamic redistribution of spin densities [4-5]. Single-molecule magnets (SMMs) stabilise high-spin ground states with strong magnetic anisotropy, leading to slow spin relaxation, large energy barriers for spin reversal, and magnetisation retention at the molecular level offering a chemically tuneable analogue to nanoscale magnetic domains [6-7]. This seminar will discuss recent results at the forefront of multifunctional molecular magnets in the context of emerging directions in the field, illustrating how molecular-level design can synergise with conventional condensed matter approaches. This perspective envisions a “bottom-up” strategy, where chemical control over spin, charge, and lattice degrees of freedom enables the construction of molecular-scale magnets with tuneable and emergent properties, bridging the molecular and solid-state realms.
References:
E. Coronado, Nat. Rev. Mater., 2020, 5, 81-104.
S. Brooker, Chem. Soc. Rev., 2015,44,2880–2892.
J. Olguín, Coord. Chem. Rev., 2020, 407, 213148
T. Tezgerevska, K.G. Alley, C. Boskovic, Coord. Chem. Rev., 2014, 268, 23−40.
A. Summers, F. Zahir, G. Turner, M. Hay, A. Riboldi-Tunnicliffe, R. Williamson, S. Bird, L. Goerigk, C. Boskovic, S. Moggach, Nat. Commun., 2024, 15(1), 8922.
V. Vieru, S. Gomez-Coca, E. Ruiz, L. F. Chibotaru, Angew. Chem., 2024, 136, e202303146
E. Moreno-Pineda and W. Wernsdorfer, Nat. Rev. Phys., 2021, 3, 645-659.