First principles calculations of transition metal complexes for artificial photosynthesis

Abstract

Nanoscale devices using transition metals have shown promise in the renewable energy context for their robustness and scalability. In artificial photosynthetic devices, light harvesting molecules drive reactions which create fuel (e.g by splitting water). For optimal fuel generation efficiency a long charge transfer excited state lifetime is necessary. Additionally, an absorption peak in the visible region is required for the molecule to absorb sunlight. To investigate the absorption peak and properties associated with the excited state lifetime of light harvesting molecules, a workflow has been developed using a combination of first principles techniques and analysis code. In the development of the workflow, this study focused on a vanadium(V) oxo compound VOLF which has been experimentally synthesized by collaborators. To fully understand the properties of this light absorbing molecule, it was studied using a variety of theoretical techniques and compared to experimental results obtained by collaborators.