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和（明尼苏达大学），Neeraj Rai（密西西比州立大学），特洛伊货车沃里斯（马萨诸塞州），本斯莱特（伦敦大学学院）（剑桥大学），亚当·卡特（爱丁堡并行计算中心），Jürg Hutter（苏黎世大学）、郭毅峰（劳伦斯利弗莫尔国家实验室）、Christopher Mundy（西北太平洋国家实验室）、Joost VandeVondele（苏黎世联邦理工学院）和Rodolphe Vuilleumier（皮埃尔&玛丽居里巴黎大学）正在合作开发和实施CP 2K计算化学软件套件中的新理论方法。 这些新的方法使反应性多相系统的预测建模，包括自由能景观和产品产量，其中系统的相互作用是由科恩-沙姆密度泛函理论与货车德瓦尔斯和混合泛函描述。 马尔可夫链蒙特卡罗方法，利用智能移动与不对称的底层矩阵，如聚集体积偏差和配置偏差蒙特卡罗方法，和吉布斯系综框架的相空间的反应性的单相和多相平衡的散装和禁闭有效的探索。 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。EPSRC为英国的研究团队提供资金。通过开发适用于各种科学和工程应用中的化学过程的反应相和吸附平衡的高效准确方法，软件基础设施得到了发展。 经过广泛验证的方法将被纳入开放源码CP 2K软件套件，以供广大用户使用。 新软件可用于确定可持续化学的最佳反应条件和分离工艺。 该合作研究团队计划使用新软件来研究反应过程，以满足社会的关键需求（用于食品供应的肥料，可再生能源的燃料和环境友好的化学过程）。

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).