We give an overview about our recent work for the development of new computational approaches with focus on spectroscopy, catalysis, and design. In particular, forefront methods for ab initio molecular dynamics (AIMD) have been in the focus of our research. We have, for instance, presented computationally efficient spectroscopic approaches for the calculation of (Resonance) Raman spectra, the first vibrational Raman optical activity spectra from AIMD for the investigation of chiral compounds as well as an AIMD approach for sum frequency generation at a semiconductor surface. In addition, efficient methods - based on, e.g., periodic density functional theory embedding – for the analysis of complex systems have been developed. Another research direction is the development of improved approaches for study and design of functional systems, in particular for catalysis. Here, we have focused on solar light-driven water splitting as a promising solution for sustainable energy storage and conversion. One of the main limiting steps in artificial water splitting is the water oxidation. In collaboration with experimentalists, we have presented the first Co(II)-cubane water oxidation catalysts, which are some of the rare stable and active artificial cubane catalysts for water oxidation. Our computational approaches have dealt with the calculation of reaction mechanisms including free energies and barriers via AIMD methods (using, for instance, enhanced sampling techniques such as metadynamics) and sophisticated consideration of environmental and solvent effects. For electronic structure beyond density functional theory, we have used wavefunction-based methods in order to obtain an improved description of involved transition metal-based catalysts. Our calculations revealed essential knowledge about factors influencing stability and catalytic activity and has paved the way for new structure-activity relationships and informed in silico design of novel water oxidation catalysts.

Advancing computational methods for spectroscopy, catalysis, and design

2019 Spring National Meeting

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