Adaptive Subsystem Density Functional Theory
Adaptive Subsystem Density Functional Theory
复制标题
自适应子系统密度泛函理论
DOI：
10.1021/acs.jctc.2c00698
复制
发表时间：
2022
影响因子：
5.5
通讯作者：
Pavanello, Michele
中科院分区：
文献类型：
--
作者：
Shao, Xuecheng;Lopez, Andres Cifuentes;Khan Musa, Md Rajib;Nouri, Mohammad Reza;Pavanello, Michele
子系统密度泛函理论（DFT）是一种用于大规模模拟分子凝聚相和界面的强有力的电子结构方法。其计算效率的关键是使用近似的非加性非相互作用动能泛函。不幸的是，目前可用的非加性泛函在子系统强烈相互作用时（例如当它们参与化学反应时）会导致不准确的结果。这项工作通过设计一个工作流来打破现状，该工作流将子系统DFT的适用性扩展到强交互子系统。这是通过在几何优化或从头算分子动力学模拟过程中实现子系统的全自动自适应定义来实现的。该方法利用现代并行化策略和面向对象编程，以一种有效的方式对子系统合并和拆分事件进行资源（包括工作和数据）的重新分配。我们用例子展示了从中等到强烈的子系统间相互作用的方法，打开了使用子系统DFT来模拟分子凝聚相化学反应的大门。
Subsystem density functional theory (DFT) is emerging as a powerful electronic structure method for large-scale simulations of molecular condensed phases and interfaces. Key to its computational efficiency is the use of approximate nonadditive noninteracting kinetic energy functionals. Unfortunately, currently available nonadditive functionals lead to inaccurate results when the subsystems interact strongly such as when they engage in chemical reactions. This work disrupts the status quo by devising a workflow that extends subsystem DFT’s applicability also to strongly interacting subsystems. This is achieved by implementing a fully automated adaptive definition of subsystems which is realized during geometry optimizations or ab initio molecular dynamics simulations. The new method prescribes subsystem merging and splitting events redistributing the resources (both for work and data) in an efficient way making use of modern parallelization strategies and object-oriented programming. We showcase the method with examples probing from moderate-to-strong inter-subsystem interactions, opening the door to using subsystem DFT for modeling chemical reactions in molecular condensed phases with a black box computational tool.