SI2-CHE: Collaborative Research: Developing First Principles Monte Carlo Methods for Reactive Phase and Sorption Equilibria in 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 Voorhis（麻省理工学院）、Ben Slater（伦敦大学学院）、michael Sprik（剑桥大学）、Adam Carter（爱丁堡并行计算中心）、j<s:1> rg Hutter（苏黎世大学）、I-Feng 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）组成的国际研究团队。Joost VandeVondele（苏黎世联邦理工学院）和Rodolphe Vuilleumier（巴黎皮埃尔和玛丽居里大学）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。这些新方法能够对反应性多相系统进行预测建模，包括自由能景观和产物产量，其中系统相互作用由Kohn-Sham密度泛函数理论与范德华和混合泛函数描述。利用具有不对称基础矩阵的智能移动的马尔可夫链蒙特卡罗方法，如聚集-体积-偏置和构型-偏置蒙特卡罗方法，以及Gibbs系综框架被用于有效地探索体和约束中反应性单相和多相平衡的相空间。美国的研究团队得到了MPS化学部门和网络基础设施办公室的联合支持。英国研究团队的资金由EPSRC提供。软件基础设施的发展是有效和准确的方法的反应相和吸附平衡，适用于各种科学和工程应用的化学过程。广泛验证的方法将被合并到开源CP2K软件套件中，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软件来研究反应过程，以解决社会的关键需求（食品供应的肥料，可再生能源的燃料，以及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 &amp; 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).