Grant: Discovery Grants Program - Individual

Chemical systems and materials are inherently complex, yet quantum chemistry requires drastic simplifications in order to build manageable models. There is an inherent tension between these aspects, and much of my research program aims at recovering some of the complexity. The proposed research is thus at the forefront of theoretical and computational chemistry. This research area applies the principles of quantum mechanics that govern the behavior of atoms, electrons and molecules to the study of chemical and materials problems. For heavy element compounds, the effects of relativity need to be added as well. My program comprises both, fundamental and applied research. Understanding beyond mere numbers is increasingly important (as it leads to insight and new, widely applicable models that in turn enable broad impact on diverse research communities); it is a driving principle for my research. Thus, I propose chemically meaningful concepts and models , e.g. regarding the nature of chemical bonds, and how they influence desired properties, or the "superatom" model for binding in clusters and molecules. Long-term goals within this framework are: (1) develop a solid understanding of actinide chemistry from theory alone; (2) achieve molecular-level understanding of the environmental chemistry of contaminants; (3) develop and characterize novel functional materials; (4) develop new computational chemistry methodology. Within this grant, my HQP and I will mainly pursue the following specific objectives: Goal 1: Study complexes of heavy metals for future use in "targeted alpha therapy" (TAT). For TAT to work, the radionuclide (225-Ac and others) needs to be strongly held - this is where we contribute, in collaboration with experimental collaborators. Incidentally, this also provides a beautiful example how prior fundamental research can inform and guide applied research in unexpected ways! Goal 2: Study interactions of radioactive actinides with biomolecules (proteins) and mineral surfaces, with a particular focus on complex features such as edges and corners. Goal 3: Understand interactions of crude oil components with ice surfaces (oil spills). Goal 4: We are broadly interested in materials chemistry: Propose polymers as support for two-dimensional (2D) materials, novel composite 2D materials, and a unique approach to "singlet fission" (a novel paradigm for solar energy conversion); focus on a range of important surface-catalyzed reactions, noting that heterogenous catalysis (catalysis on surfaces) is of crucial industrial importance. We will prove the - so far largely overlooked - importance of extended surface features (e.g. edges) for these reactions, proposing a novel paradigm. Goal 5: Develop a new method for inclusion of solvation effects into computational-chemistry studies of molecules and materials. Moreover, we will develop new, innovative approaches and models to tackle chemical complexity, such as for surface reactivity.