Reduced Scaling Many-Body Electronic Structure Methods: Improved Accuracy and Precision

缩小比例的多体电子结构方法：提高准确性和精度

基本信息

批准号：
1800348
负责人：
Edward Valeev
金额：
$ 45万
依托单位：
Virginia Polytechnic Institute and State University
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2018
资助国家：
美国
起止时间：
2018-07-15 至 2022-06-30
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1800348&HistoricalAwards=false
关键词：
Reduced Scaling Many Body Electronic

项目摘要

Edward Valeev of Virginia Polytechnic Institute and State University is supported by an award from the Chemical Theory, Models and Computational Methods Program in the Chemistry Division to develop efficient and accurate methods for studying the electronic properties of large molecules, crystalline solids, and interfaces. It is possible to predict the properties of matter around us by applying the laws of quantum mechanics to describe the behavior of electrons in atoms, molecules, and solids. Unfortunately, exact computational and theoretical modeling of electron behavior in systems with more than a few atoms is beyond the ability of even the most powerful supercomputers currently available due to the steep increase of computational cost with the number of electrons. Valeev and co-workers are developing methods that reduce the computational cost of accurate calculations by many orders of magnitude and make predictive simulations possible for systems with thousands of atoms. Such advances are crucial for our ability to design molecules and materials for particular functions, such as creating new catalysts for converting solar light into fuel. The methods developed are being included in widely-used software packages that may enhance research capabilities for national and international researchers.This project focuses on the development of many-body electronic structure methods (such as the diagrammatic perturbation theory and coupled-cluster) with reduced scaling with respect to system size (by exploiting low-rank and sparse structure of the operators and states) and precision (by building in the correct analytic structure via explicit correlation). This development builds upon recent advances by Valeev and co-workers that demonstrated that complete basis set coupled-cluster with singles, doubles, and perturbative triples calculations could be performed on closed-shell molecules with more than a thousand atoms. This project extends the approach to the treatment of molecules with open-shell electronic states, to manifolds of electronic states, and to electronic states of crystalline solids. The efficiency of the rank compression is being improved by tailoring representations to the particular electronic structure model. Lastly, the project applies these ideas to the high-order coupled-cluster models to extend their applicability to systems with 30-50 atoms. In addition to making these codes available through a widely-used software package, the work being done provides excellent training for graduate students and postdoctoral fellows.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

弗吉尼亚理工学院和州立大学的爱德华·瓦利夫（Edward Valeev）得到了化学理论，模型和计算方法计划的奖项，以开发有效，准确的方法来研究大分子，结晶固体和界面的电子特性。可以通过应用量子力学定律来描述原子，分子和固体中电子的行为来预测我们周围物质的特性。不幸的是，由于电子数量的急剧增加，电子行为在具有多个原子的系统中对电子行为的精确计算和理论建模超出了当前可用的最强大的超级计算机的能力，这是由于电子数量急剧增加。 Valeev和同事正在开发将准确计算的计算成本降低的数量级，并使具有数千原子的系统的预测模拟成为可能。这种进步对于我们设计特定功能的分子和材料的能力至关重要，例如创建将太阳能转换为燃料的新催化剂。所开发的方法包括在广泛使用的软件包中，可以增强国家和国际研究人员的研究能力。本项目着重于发展多体电子结构方法（例如图解摄动理论和耦合群集）的多体电子结构方法（例如，通过降低了尺寸的缩放（通过较低的型号）（通过较低的型结构）（通过较低的状态结构）（通过较低的状态结构）（通过较低的状态结构）进行纠正（并构建状态），并且相关性）。这一发展是建立在Valeev和同事的最新进展基础上的，这些进步表明，可以在具有超过一千个原子的封闭壳分子上进行完整的基础耦合群集与单打，双打和扰动三元的计算。该项目扩展了用开放式电子状态，电子状态的流形和晶体固体的电子状态的分子处理方法。通过根据特定电子结构模型调整表示形式来提高等级压缩的效率。最后，该项目将这些想法应用于高阶耦合群集模型，以将其适用性扩展到具有30-50个原子的系统。除了通过广泛使用的软件包提供这些代码外，所完成的工作还为研究生和博士后研究员提供了出色的培训。该奖项反映了NSF的法定任务，并被认为是通过基金会的知识分子的智力优点和更广泛影响的评估审查标准来通过评估来获得支持的。