Embedded Cluster Modelling for Realistic Solid-State Systems

The combination of computer simulation with experiment is fundamental to achieving new understanding in chemistry, and to delivering advances that can address the most pressing societal challenges. The integration of computer simulation into research across the chemical sciences has been accelerated by the accessibility of high-performance computing infrastructure and tailored software that can harness the distributed architectures.

New materials and chemical processes can be predicted by models of atoms and electrons using this infrastructure, with periodic density functional theory (DFT) at the forefront of the field of applied materials simulation. However, the efficacy of these modelling paradigms is proportional to the degrees of freedom in the system, which means that big models with lots of electrons, such as when considering catalytic processes, become very expensive to simulate.

To address these shortcomings, this Fellowship looks to improve the capability and accessibility of methods that can provide high-level accuracy for electronic structure simulations, necessary for bond-breaking or bond-forming reactions, with reduced degrees of freedom, which means simulations can be performed quicker.

This Fellowship is delivering new multiscale modelling paradigms, and the aim of this renewal is to make these paradigms more accessible through easier to use frameworks, and to extend our capabilities by integrating new machine-learning models into the simulation workflow, with the potential for acceleration in accurately resolving aspects of the system wavefunction. The new capabilities will continue to be developed in internationally leading software packages (FHI-aims, ChemShell) with collaborative partners distributed globally in academia and government research laboratories.

The Fellowship will simultaneously look to demonstrate the potential of these new methods, with aims to resolve key mechanistic aspects of the synthesis of renewable fuel in collaboration with experimental partners in academia, notably at the host institution (Cardiff Catalysis Institute, Cardiff University) and via collaborations through the UK Catalysis Hub, as well as industry (Johnson Matthey, bp). The Fellowship aims to provide new knowledge of how the catalytic active site structure defines reactivity and selectivity in processes relating to photo- and electro-catalytic H2 generation; and also to explore how the structure of support materials influences thermally driven catalytic transformation of waste to sustainable aviation fuel.

Finally, the Fellowship has complementary aims to support the transition of the research team from emergent researchers to influential and authoritative research leaders who can support the development of both new research domains and the next generation of researchers. The research team will be supported in developing, practising, and reflecting on their leadership activities, so they can deliver lasting impact in their sphere of influence.