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

SI2-CHE：协作研究：在 CP2K 软件套件中开发反应相和吸附平衡的第一原理蒙特卡罗方法

• 批准号: 1265849
• 负责人: Joern Ilja Siepmann
• 金额: $ 34.93万
• 依托单位: University of Minnesota-Twin Cities
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2013
• 资助国家: 美国
• 起止时间: 2013-04-15 至 2017-03-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1265849&HistoricalAwards=false
• 关键词: SI2; CHE; Collaborative; Research; Developing

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).

由Ilja Siepmann，Ben Lynch（明尼苏达大学），Neeraj Rai（密西西比州立大学），Troy Van Voorhis（马萨诸塞州技术学院），本·斯莱特（Ben Slater）（伦敦大学学院），米歇尔·斯普里克（Michiel Sprik）（剑桥大学），亚当·卡特尔（Adam Carter）（爱丁堡平行中心（Edinburgh Partelling Center）（iinforggh anflice Center）， Kuo（Lawrence Livermore国家实验室），Christopher Mundy（Pacific Northwest National Laboratory），Joost Vandevondele（Eth Zurich）和Rodolphe Vuilleumier（Pierre＆Marie Curie Paris大学）正在合作开发和实施CP2K Computicational Computicational Chemical Compational Chemical Chemical Chemation Compational Chemation Compational Chemation Compational Chemation Compation Atchemational Compation Atchemation Compation Atchemational。这些新方法可以实现反应性多相系统的预测建模，包括自由能景观和产品产量，其中系统相互作用由Kohn-Sham密度功能理论与Van der Waals和Hybrid功能进行描述。马尔可夫链蒙特卡洛（Monte Carlo）使用智能动作采用了不对称的潜在物质，例如聚集体积偏见和构型偏见蒙特卡洛方法，以及吉布斯集合框架用于有效地探索反应性单相和多相的相位空间。美国的研究团队得到了国会议员的化学部和网络潮流办公室的共同支持。 EPSRC提供了基于英国的研究团队的资金。软件基础架构是通过开发有效，准确的方法来进行反应阶段和吸附等效物，这些方法适用于潜水科学和工程应用中的化学过程。经过广泛验证的方法将合并到开源CP2K软件套件中，以使其可用于大型用户群。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。协作研究团队计划使用新软件来调查应对社会关键需求的反应性过程（食品供应的肥料，可再生资源的燃料以及环境良性的化学过程）。