Collaborative Research: SI2-CHE:Developing First Principles Monte Carlo Methods for Reactive Phase and Sorption Equilibria in the CP2k Software Suite

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An international research team consisting of Ilja Siepmann, Ben Lynch (University of Minnesota), Neeraj Rai (Mississippi State University), Troy Van Voorhis (Massachusetts Institute of Technology), Ben Slater (University College London), Michiel Sprik (University of Cambridge), Adam Carter (Edinburgh Parallel Computing Centre), Jürg Hutter (University of Zurich), I-Feng Kuo (Lawrence Livermore National Laboratory), Christopher Mundy (Pacific Northwest National Laboratory), Joost VandeVondele (ETH Zurich), and Rodolphe Vuilleumier (University Pierre & Marie Curie Paris) is collaborating to develop and implement new theoretical methods in the CP2K computational chemistry software suite. These new methodologies enable the predictive modeling of reactive multi-phase systems, including free energy landscapes and product yields, where the system interactions are described by Kohn-Sham density functional theory with van der Waals and hybrid functionals. Markov chain Monte Carlo approaches utilizing smart moves with asymmetric underlying matrices, such as the aggregation-volume-bias and configurational-bias Monte Carlo methods, and the Gibbs ensemble framework are employed for efficient exploration of the phase space for reactive single- and multi-phase equilibria in bulk and in confinement. The U.S. based research team is supported jointly by the Chemistry Division in MPS and the Office of Cyberinfrastucture. Funds for the UK based research team are provided by the EPSRC.The software infrastructure is advanced by the development of efficient and accurate methodologies for reactive phase and sorption equilibria that are applicable to chemical processes in diverse science and engineering applications. The extensively validated methodologies will be incorporated into the open-source CP2K software suite to make them available to a large user base. The new software can be used to identify optimal reaction conditions and separation processes for sustainable chemistry. The collaborative research team plans to use the new software for the investigation of reactive processes that address critical needs of society (fertilizers for food supply, fuels from renewable sources, and environmentally benign chemical processes).