Scalable Quantum Chemistry with Flexible Embedding

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We propose to develop and a new piece of software for molecular modelling of reactivity in complex systems, in particular, surface chemistry and heterogeneous catalysis in the presence of solvent such as water.Examples of the science we are targetting are * metal oxide catalysis that work in the presence or water * the binding of pollutant species (heavy metals or toxic organics) to natural minerals in the environment, or specially designed inorganic materials that could potentially remove them from the environment * catalysis by more complex minerals, not well treated by existing treatments but of great industrial importance * design of sensors and photoelectric materials by organic layers on inorganic surfacesWe will do this by combining quantum chemistry (also known as first principles) techniques, which can treat the chemically reacting centres with classical (or empirical) models for the rest of the system (the slab of material which is modelling a surgfae, and the solvent layers on top of it.The novelty in our approach is that we are extending the quality of the interaction between the classically modelled environment and the quantum mechanical calculation in a number of significant respects. We are combining some of our own ideas, such as adapting existing models to include spin polarisation effects with ideas (frozen electron density models for water molecules) that have been developed and tested by others.We are choosing an Open Source quantum chemistry program, NWChem as the basis for the new features because it has been designed from scratch for use on high-performance computers, and is modular in design which will help support the changes we need to make. The MM code (GULP) is already used in our existing work, and works well on parallel machines. Parallel efficiency is a key driver for the design of the interfaced code and will inform the way we implement the new methods.In the long run, it is intended the code developed here will form the nucleus of a modelling framework for a wider range of systems (including biological ones) building on experience we have had in past software projects (www.chemshell.org).