Ab initio modelling of photoinduced electron dynamics in nanostructures

In particular, two-dimensional (atomically thin) materials such as transition metal dichalcogenides (TMDs) have been extensively researched and shown to exhibit, e.g., strong optical absorption when compared to their bulk counterparts, with potential applications in photovoltaics for solar energy.

The optical absorption in such materials may be further improved by decoration with metal nanoparticles (MNPs) due to a plasmonic enhancement effect. While such an effect has been demonstrated experimentally, it is hard to show theoretically from an ab initio point of view due to the computational demand of such calculations: the state-of- the-art approaches commonly used to determine the optical spectra of, e.g, the semiconducting TMD (i.e. density functional theory (DFT) and many-body perturbation theory) may not be applied to the full TMD-MNP structure as the MNP is often on a much larger scale than the semiconductor rendering the ab initio methods infeasible.<br><br>In this thesis, we develop a dynamical, hybrid approach (the projected equations of motion (PEOM) method) where a composite material is split into subsystems which are then coupled electromagnetically.