Beyond the static description of the electronic structure:Excited state dynamics in transition metal complexes and organic compounds

Identifier:  TDX:3173

Handle: https://hdl.handle.net/20.500.11797/TDX3173

Authors:  Alías Rodríguez, Marc

Abstract:
The description of the excited states is important to rationalize processes happening after irradiation of light. The comprehension of them is an important tool to tune materials for different applications. In previous studies in our group, these descriptions were limited to a static calculation of the electronic structure for the involved states. In this thesis, we have gone one step further to describe these processes from a dynamic point of view through three different methodologies. The first method employed has been the time-dependent Fermi's golden rule in two iron (II) complexes. This method has been proved to accurately determine the intersystem crossing rates and lifetimes in relatively fast processes. However, this gives unphysical rates in the study of an ultra-fast process. This last process is also studied with nuclear quantum dynamics by means of Multi-Configuration time-dependent Hartree (MCTDH). This second methodology needs the creation a priory of a model Hamiltonian and has been used in the reverse-LIESST process of an iron (II) complex and the ultrafast triplet population in xanthone molecule.