Non-adiabatic quantum molecular dynamics of complex systems

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Non-adiabatic transitions and quantum mechanical tunneling of protons are important processes in chemical and biochemical systems. The description of such processes in complex systems using non-adiabatic quantum dynamics methods is the aim of this project. In the last decade the ring-polymer molecular dynamics (RPMD) approach has shown to be a useful tool for approximate quantum dynamics simulations. Non-adiabatic processes cannot be described using the RPMD approach directly, but an extension of the RPMD approach to simulate two-state non-adiabatic processes, the kinetically constrained (KC) RPMD, was proposed very recently. The project aims to generalize and further develop the KC-RPMD approach. Furthermore, the approach will be used to investigate chemically and biochemically important non-adiabatic processes in complex systems. Several bioinorganic systems showing electron transfer processes (ET) or proton coupled electron transfer processes (PCET) can be considered: complexes based on Bis(imidazole) Iron Tetraphenylporphyrins, azurin proteins, a tris(phosphine)borane-supported iron complex, iron complexes with tris(phosphino)alkyl ligands featuring an axial carbon donor, cobalt complexes with diglyoxime ligands.