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，因为我们纯粹通过模拟来预测分子和材料的性质的能力越来越强。当分子与固体表面相遇时，这一点尤其正确--因为在这样的环境下进行实验的特殊挑战。然而，表面分子前沿包含了一大类具有巨大实际重要性的问题：据估计，表面工艺促进的工业应用在全球生产了价值超过15万亿美元的商品和产品。这项研究将通过扩展最初由开发的用于模拟分子中电子的先进模拟方法来提高我们在表面模拟分子物理和化学的能力。该项目不仅将促进我们对表面科学的基本理解，而且还将为与生产和储存清洁能源以及设计改进的催化剂相关的技术应用开辟一条道路。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。该软件将是对美国网络基础设施的独特贡献，并激励美国和世界各地的其他研究人员进一步创新，他们将能够免费获取其源代码。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。一个前沿的模拟挑战存在于化学和材料科学的两个领域的交叉点-即以预测的准确性确定固体表面上分子的性质和化学。表面分子的前沿包括一大类具有巨大实际意义的问题：多相催化、光伏和新兴的电子材料。然而，从模拟的角度来看，目前还不可能有效地将高精度多体分子和周期凝聚相方法的最新进展结合在这些问题上，因为分子和材料的电子结构理论之间存在着巨大的差距，这反映在不同的算法和不相交的代码库中。该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在理论、算法和可用的社区软件实施方面的差距。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，该软件框架将允许在同等基础上准确计算分子和固体的第一原理电子结构-并具有高通量筛选或从头计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放源码量子化学软件以及自动化计算机实施和高性能并行库方面的领先记录的基础上。该项目将使分子电子结构-嵌入、缩小尺度多体方法、精确激发态电子结构等-的进展可以常规地应用于与表面化学相关的分子、材料和两者的组合。这将极大地促进电子结构处理的最先进水平，并开辟新的理论探索路线。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。基于美国的开源先进材料代码是美国网络基础设施中的一个长期遗漏。作为以前所未有的精度模拟分子、固体及其界面电子结构的高性能框架，EMOS将对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重用与其他主要的电子结构组件集成在一起。该项目将为学生和博士后提供宝贵的培训机会，他们将在首席调查人员的直接监督下开发软件框架。此外，每个项目点都将通过每年夏天接待代表更广泛理论界的来访学生和教职员工，对他们进行关于在研究和教育中使用EMOS的培训，从而促进EMOS利益攸关方网络的发展。项目组还将在这一领域已有努力的基础上，在教学班级和暑期学校中使用EMOS；这些努力还将扩展到网上环境。

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.