Chemistry is the science of matter and its transformation. Ideally, chemical transformations should yield the desired products at minimum energy consumption and waste generation. Catalysts are essential to achieve this goal, see the figure above. To understand and to control chemical transformations and catalytic processes are key to developing sustainable energy technologies. Computation is a valuable tool for understanding chemical transformations [1, 2]. However, synergy between experiment and computation is often hampered by lack of detailed experimental data and incomplete theoretical exploration of the chemical systems. The improved resolution of new light sources will allow exploration of key steps on the time scale of chemical processes, producing a wealth of new experimental data. A complete understanding of these processes will require theoretical analysis with adequate protocols and methods. To match these experimental developments, we will improve the theoretical description by combining state-of-the-art electronic-structure and multiscaling methods with new techniques for automatic reaction-space exploration such as the Global-Reaction-Route-Mapping (GRRM) method [3]. Electronic, vibrational, and NMR data generated using, for instance, the relativistic methods of RT1 and the functionality of OPENRSP will be employed for direct comparison of theoretical predictions and experimental observations, facilitating the understanding of current systems and the development of improved catalysts.
Fourth-generation light sources will open two highly challenging avenues of research, for which novel computational strategies must be developed—namely, the control of chemical reactivity and the control of energy transfer. The control of reactivity, stability, and selectivity by structural elements, pressure, fields, or pulses is the holy grail of catalytic design. To make breakthroughs in reaction control, we will develop computational strategies incorporating the methods of RT1–RT3 for an accurate treatment of molecules and their reaction pathways in complex environments and in the presence of fields, spurring new experimental work by our collaborators. Second, chemical transformations for sustainable energy technologies or for the transformation of unreactive molecules such as CO2 into added-value chemicals will not only require an understanding of energy conversion and transportation in the reactive system itself but also of the transfer of energy to the environment. The most efficient conversion mechanisms in nature use complex interactions with the environment to convert, for instance, solar light into chemical energy. The design of such processes is a formidable task, requiring an understanding of electronic correlation, of conversion of energy into vibrational degrees of freedom at the femtosecond scale, and of energy dissipation at longer time scales.
Combining reaction-space exploration with methods for multicomponent reactions and matter–field interactions emerging from RT1–RT3, we will be able to analyse systems currently beyond reach and to design novel, efficient catalysts, initially benefiting from two RCN Young Research Talent (YRT) grants (Hopmann, Nova) and one MSCA Career Integration Grant (CIG) (Balcells).
[1] K. H. Hopmann. “Quantum chemical studies of asymmetric reactions: Historical aspects and recent examples”. Int. J. Quantum Chem. 115 (2015), 1232. [2] D. Balcells et al. “Deciphering selectivity in organic reactions: a multifaceted problem”. Acc. Chem. Res. 49 (2016), 1070. [3] K. Ohno et al. Global Reaction Route Mapping. URL: http://grrm.chem.tohoku.ac.jp/ GRRM/index_e.html.