SMMs are compounds that present magnetic memory effects of pure molecular origin and as such are being investigated for high-density information storage devices. In the last few years, the field has witnessed an astonishing progress, with working temperatures going past the liquid nitrogen limit. Some of my recent contributions to this multidisciplinary field are listed below.
In this paper we report a series of dinuclear lanthanide compounds (Gd, Tb, Dy) that interact strongly through a delocalised d-type orbital. Dy-based compound presents open magnetic hysteresis (coercive field of 14 T) at temperatures as high as 60 kelvin.
J. Am. Chem. Soc. 2021, 143, 15, 5943–5950.
In this paper we applied the ab initio spin dynamics methodology, developed within the Chilton Group, to the best performing SMMs reported so far and identified the most important factors that determine their differing magnetic properties. Using this knowledge, we investigated a series of hypothetical compounds revealing that the figure of merit commonly adopted in the community cannot be further optimised, which highlights the need for new design criteria based on spin-phonon engineering.
This landmark study presented the first example of a Dysprosium atom sandwiched between two cyclopentadienyl ligands, leading to an extraordinarily large axial crystal field and record-breaking magnetic properties. Led by Chilton, we put forward a theoretical and computational framework that described, for the first time, the spin dynamics of a SMM from first principles.
