Expanding the range of computational quantum chemistry: actinide molecular science and solid-state chemistry

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My research program falls into the general area of computational and quantum chemistry. The growing relevance of this field has been recognized with the 1998 Nobel Prize in Chemistry that has been awarded to W. Kohn and the late J. Pople, two outstanding pioneers of the field. Within this framework, the principal, long-term goals of my research are twofold.First, computational quantum chemistry has reached a point where it can be used by chemists as one of several standard, "black-box" approaches for solving certain problems. This is the case for instance for organic chemistry of small and medium-sized molecules. Yet, the same kind of maturity has not been reached in other areas. My first goal, then, is to develop computational quantum chemistry methods into valuable and reliable research tools for areas where they have not yet reached their full potential. One such area concerns modeling of extended systems (solids, surfaces, etc.), where my group will develop extensive new quantum-chemical methods for the simulation of nuclear magnetic resonance (NMR) and electron spin resonance (ESR) parameters. Another area comprises the chemistry of the heaviest parts of the periodic table, the actinide elements. These elements present unique challenges to the researcher. Here, I will build on a range of existing local and international collaborations to develop new methods (chiefly concerning relativistic effects) and to apply and test methods that have not been used in this connection.As the second principal research goal, I aim at developing a solid understanding of the chemistry of the actinide elements (uranium, neptunium, plutonium, among others) from theory and computations alone, so as to avoid difficult and dangerous experiments with radioactive materials as much as possible. In this field, which can be described as "theoretical actinide molecular science", I will focus on modelling molecules in aqueous solution as well as selective extraction agents and related complexes. These are systems that are relevant to the nuclear waste problem at contaminated sites (for instance, uranium mine tailings in Canada's North).