As the researcher was offered an independent research position, the project was formally terminated after nine months, so that not all goals anticipated for the initial 24-month funding period were achieved. The electronic structure of existing dinitrogen photocleavage catalysts were described at several levels of theory, including density functional theory, complete active space self consistent field and density matrix renormalization group methods. Adequate levels of theory to describe the different complexes of interest were found and validated by comparing predicted observables with experimental data, e.g. geometries and electronic absorption spectra.
The analysis of the thus obtained electronic structure descriptions of the known dinitrogen photocleavage catalysts permitted initial insights into their working principles, e.g. the characterization of the electronic excitations that are responsible for dinitrogen photocleavage. It was also found that a full picture of the excited state decay and the fundamental reasons behind competitive nitrogen-nitrogen and metal-nitrogen bond cleavage will only be unraveled from dynamical simulations. These simulations were prepared, and the researcher and the host will continue a collaboration to finalize this project.
The preliminary results were disseminated to the scientific community at three conferences so far. Future dissemination of the results will include further presentations at conferences as well as the publication in open-access journals to ensure that the results are available to a broad audience.
