Magnetic Molecules: structure, spectroscopy, and dynamics


Jon Kragskow




Donostia International Physics Center (Hybrid Seminar)


Daniel Reta

An understanding of how the properties of molecules and materials are influenced by chemical structure is key to the rational design of novel systems and devices. One such example is electron-phonon coupling (EPC), where electronic structure is modulated over time by vibrational motion, and is the driving force behind processes such as non-radiative decay in luminescent materials and light absorbing proteins, transport in batteries and energy conversion devices, loss of magnetisation in magnetic materials, and qubit decoherence in quantum computing, In recent years, molecular and solid-state simulations of EPC have improved vastly, while the spectroscopic experiments required to directly measure this phenomenon, and to benchmark EPC calculations, remain rare. Two examples of such spectroscopic approaches are the Far-Infrared and Raman MagnetoSpectroscopy (FIRMS/RaMS) techniques which combine sensitive IR and Raman spectroscopy measurements with magnetic fields (0-17 T), allowing for the direct observation of electron-phonon coupled signals. A few years ago, we presented the first fully ab initio simulation of a FIRMS experiment, and in doing so were able to link structural and symmetry elements to the presence of specific spectral features, and to confirm the accuracy of our ab initio EPC calculations. This talk will discuss the need for the FIRMS and RaMS methods, the development and theory of the methods used to model them, and an example of their application to a lanthanide molecular spin qubit.