SI2-CHE: Collaborative Research: Developing First Principles Monte Carlo Methods for Reactive Phase and Sorption Equilibria in the CP2K Software Suite

由Ilja Siepmann、Ben Lynch(明尼苏达大学)、Neeraj Rai(密西西比州立大学)、Troy Van Voorhim(麻省理工学院)、Ben Slatk(伦敦大学学院)、Michiel Sprik(剑桥大学)、Adam Carter(爱丁堡并行计算中心)、Jürg Hutter(苏黎世大学)、I-峰Kuo(劳伦斯·利弗莫尔国家实验室)、Christopher Mundy(太平洋西北国家实验室)、Joost VandeVondele(苏黎世ETH)和Rodolphe Vuilleumier(巴黎大学Pierre&Amp；Marie Curie Paris)组成的国际研究团队正在合作开发和实施CP2K计算化学软件套件中的新理论方法。这些新的方法使得对反应多相系统的预测建模成为可能，包括自由能景观和产物产率，其中系统的相互作用由Kohn-Sham密度泛函理论和van der Waals和混合泛函描述。马尔可夫链蒙特卡罗方法利用具有非对称标的矩阵的智能移动，如聚集体积偏置和构型偏置蒙特卡罗方法，以及Gibbs系综框架，用于有效地探索体相和禁闭中反应性单相和多相平衡的相空间。总部设在美国的研究小组得到了MPS化学部和网络基础设施办公室的联合支持。总部设在英国的研究团队的资金由EPSRC提供。软件基础设施是通过开发适用于不同科学和工程应用中的化学过程的高效和准确的反应相和吸附平衡方法来推进的。经过广泛验证的方法将被合并到开源CP2K软件套件中，以使其可供大量用户使用。新软件可用于确定可持续化学的最佳反应条件和分离过程。合作研究小组计划使用新的软件调查满足社会关键需求的反应过程(食品供应的化肥、可再生来源的燃料和无害环境的化学过程)。

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).