Collaborative Research: SI2-SSI: Software Framework for Electronic Structure of Molecules and Solids

许多传统的实验学科，如化学和材料科学正在迅速变化，因为我们越来越有能力纯粹通过模拟来预测分子和材料的性质。当分子遇到固体表面时尤其如此-这是由于在这种环境中进行实验的特殊挑战。然而，表面分子前沿包含了大量具有巨大实际意义的问题：表面过程促进的工业应用估计在全球生产价值超过15万亿美元的商品和产品。 这项研究将提高我们模拟表面上分子的物理和化学的能力，通过扩展最初为模拟分子中的电子而开发的先进模拟方法。该项目不仅将推进我们对表面科学的基本理解，还将为生产和储存清洁能源以及设计改进的催化剂的技术应用开辟道路。这项研究可能会产生一种新的计算机软件框架，用于模拟分子和材料中的电子。该软件将为美国网络基础设施做出独特的贡献，并刺激美国和世界各地的其他研究人员进一步创新，他们将能够免费访问其源代码。该软件框架还将作为培训计算化学家和材料科学家的教育平台。前沿模拟挑战在于化学和材料科学两个领域的交叉点-即以预测精度确定固体表面上分子的性质和化学性质。表面分子的前沿领域包含了大量具有巨大实际意义的问题：多相催化、光催化和新兴的电子材料。然而，从模拟的角度来看，它是目前不可能有效地结合联合收割机在这些问题中的高度准确的多体分子和周期性凝聚相方法的最新进展，由于如何制定分子和材料的电子结构理论之间的显着差距，反映在不同的算法和不相交的代码库。这个项目的目标是减少和/或完全消除分子和固态电子结构方法之间的差距，在理论上，算法，并在可用的社区软件实现。这将通过建立一个雄心勃勃的分子和固体电子结构（EMOS）软件框架来实现，该框架将允许在同等基础上精确计算分子和固体的第一原理电子结构-并且具有高通量筛选或从头算分子动力学所需的高效率。这些努力建立在主要研究人员在开发开源量子化学软件以及自动化计算机实现和高性能并行库方面的领先记录之上。该项目将允许从分子电子结构的进步-嵌入，缩小规模的多体方法，精确的激发态电子结构等-被常规应用于分子，材料，以及与表面化学相关的两者的组合。这有很大的潜力，以推进国家的最先进的治疗电子结构和开辟新的路线的理论研究。由此产生的开源生产质量工具包将根据大量表面现象的实验数据进行验证，从激子动力学到表面光谱和催化。一个开源的美国先进材料代码是美国网络基础设施中长期存在的一个遗漏。EMOS作为一个高性能的框架，以前所未有的精度模拟分子、固体及其界面的电子结构，将为这一努力做出重大贡献。此外，基于模块化组件的结构将能够通过模块的再利用与其他主要电子结构包集成。该项目将为学生和博士后提供宝贵的培训机会，他们将在主要研究人员的直接监督下开发软件框架。此外，每个项目地点将通过每年夏天接待代表更广泛的理论界的访问学生和教师，对他们进行在研究和教育中使用EMOS的培训，为EMOS利益攸关方网络的发展做出贡献。项目小组还将在这一领域已经开展的工作的基础上，在教学班和暑期学校中使用EMOS;这些工作还将扩展到在线环境。

Many traditionally experimental disciplines such as chemistry and materials science are rapidly changing due to our increasing ability to predict properties of molecules and materials purely by simulation. This is particularly true when molecules meet solid surfaces - due to the particular challenges of experiments in such a setting. Yet the molecule-on-surface frontier encompasses a vast class of problems of tremendous practical importance: industrial applications facilitated by surface processes are estimated to produce globally more than than 15 trillion USD worth of goods and products. This research will improve our ability to simulate the physics and chemistry of molecules on surfaces by extending the advanced simulation methodologies that were originally developed by for modeling electrons in molecules. This project will not only advance our fundamental understanding of the surface science but also open a road to technological applications relevant to producing and storing clean energy and in designing improved catalysts. The research may result in a new computer software framework for simulating electrons in molecules and materials. This software will be a unique contribution to the U.S. cyberinfrastructure and spur further innovation by other researchers in the US and worldwide, who will be able to access its source code for free. The software framework will also serve as an education platform for training computational chemists and materials scientists.A frontier simulation challenge lies at the intersection of the two domains of chemistry and materials science - namely to determine, with predictive accuracy, the properties and chemistry of molecules on solid surfaces. The molecule-on-surface frontier encompasses a vast class of problems of tremendous practical importance: heterogeneous catalysis, photovoltaics, and emerging electronic materials. Yet, from a simulation perspective, it is not currently possible to efficiently combine the recent advances in highly accurate many-body molecular and periodic condensed phase methodologies in these problems, due to a significant gap between how the electronic structure theories of molecules and materials are formulated, as reflected in distinct algorithms and disjoint codebases. The goal of this project is to reduce and/or completely eliminate the gap between molecular and solid-state electronic structure methodologies, in theory, algorithms, and in usable community software implementations. This will be achieved by building an ambitious Electronic structure for Molecules and Solids (EMOS) software framework that will permit accurate computation of the first-principles electronic structure of both molecules and solids on an equivalent footing - and with the high efficiency necessary for high-throughput screening or ab initio molecular dynamics. These efforts build on the leading track-record of the principal investigators in developing open-source quantum chemistry software as well as automated computer implementation and high-performance parallel libraries. The project will allow the advances from molecular electronic structure - embedding, reduced-scaling many-body methodology, accurate excited-state electronic structure, and others - to be applied routinely to molecules, materials, and combinations of the two as relevant to surface chemistry. This has great potential to advance the state-of-the-art in treatment of electronic structure and open new lines of theoretical inquiry. The resulting open-source production-quality toolkit will be validated against experimental data for a host of surface phenomena, from exciton dynamics to surface spectroscopy and catalysis. An open-source US-based advanced materials code is a long-standing omission in U.S. cyberinfrastructure. As a high-performance framework for simulation of electronic structure of molecules, solids, and their interfaces with unprecedented accuracy, EMOS will be a significant contribution to this effort. Further, the modular component based structure will be able to be integrated with other major electronic structure packages through the reuse of the modules. This project will provide invaluable training opportunities to the students and postdocs who will develop the software framework under the direct supervision of principal investigators. In addition, each project site will contribute to the development of a stakeholder network for EMOS by hosting, each summer, visiting students and faculty representing the broader theoretical community, to train them on the use of EMOS in research and education. The project team will also use EMOS in teaching classes and summer schools, building on already established efforts in this area; these efforts will also be extended to an online setting.