Development of Accurate Simulation Tools for the Quantification of Chemical Reactivity in the Gigapascal Regime

• Applicant: Professor Dr. Tim Neudecker
• Subject Area: Theoretical Chemistry: Electronic Structure, Dynamics, Simulation
• Term: since 2026
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 568455617

This project aims at the development of a novel computational methodology to quantify chemical reactivity in the gigapascal range. At such high pressures, covalent bonds are compressed and softer degrees of freedom, e.g., torsions or bendings, are displaced even more tremendously. The accompanying electronic changes and the resulting decrease in volume of a substance are, at present, hardly understood at a molecular level. By combining their expertise in quantum chemical method development, Conceptual Density Functional Theory (CDFT) and the modeling of chemical reactions, the mixed German/Belgian project team will devise a novel simulation tool for high-pressure structural and volume prediction for molecular clusters, which will subsequently be used in the calculation of reactivity descriptors such as chemical hardness/softness and electrophilicity. General reactivity rules for the gigapascal range will be devised by in-depth analyses of the electronic structure of the compressed compounds and volume changes throughout the course of a pressure-induced chemical reaction. For the first time, the crucial role of the chemical environment will be investigated in detail by developing a novel embedding approach for high-pressure chemistry, allowing the ab initio calculation of experimental parameters that quantify the compressibility of substances in unprecedented detail. Such considerations are of tremendous interest in experimental high-pressure chemistry, which is usually carried out using a Diamond Anvil Cell (DAC). The extensive use of experimental benchmark data, predominantly stemming from pericyclic reactions at high pressure, will guarantee the reliability of the simulation protocol. The computational tools developed within this project will allow the rational design of pressure-driven reactions and boost our understanding of the physico-chemical processes in experimental high-pressure setups.

• DFG Programme: Research Grants
• International Connection: Belgium
• Partner Organisation: Fonds Wetenschappelijk Onderzoek - Vlaanderen ; Research Foundation Flanders (FWO)
• Cooperation Partners: Professorin Dr. Mercedes Alonso, Ph.D.; Professor Dr. Frank De Proft