CAREER: Finite Temperature Electronic Structure Methods for Predicting Material Phase Diagrams

职业：预测材料相图的有限温度电子结构方法

• 批准号: 2046744
• 负责人: Brenda Rubenstein
• 金额: $ 65万
• 依托单位: Brown University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-05-01 至 2026-04-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2046744&HistoricalAwards=false
• 关键词: CAREER; Finite; Temperature; Electronic; Structure

Brenda Rubenstein of Brown University is jointly funded by the Chemical Theory, Models and Computational Methods program in the Division of Chemistry, and the Established Program to Stimulate Competitive Research (EPSCoR) to develop new methods for modeling the finite temperature electronic properties of correlated materials. In applications ranging from catalysis to astrophysics to material science, molecules and materials can be subjected to high temperatures. Nevertheless, relatively few theories exist to predict how these materials will behave at such temperatures,thwarting our ability to engineer materials such as high-Tc superconductors and next-generation thermally-responsive technologies. As part of this project, the Rubenstein Group will develop a suite of complementary theories and simulation techniques that will enable the high-accuracy modeling of complex materials at finite temperatures. In addition to this research, the Rubenstein Group will bolster its ongoing efforts to actively mentor historically-underrepresented high school students in Rhode Island through the science fair process via the Rhode Island American Chemical Society Project SEED and Advocate Programs (which Dr. Rubenstein leads) and grant area high school students opportunities to engage in real experiments through the Brown University Chemistry Department’s STEM Day Program. Dr. Rubenstein also is developing a new Accelerating Chemical Discovery course and related textbook with the aim of familiarizing undergraduates in the chemical sciences with how data science can be leveraged to solve everyday problems in chemistry.The central aim of this proposal is to develop a suite of new finite temperature electronic structure techniques to elucidate the electronic phase diagrams of correlated materials. In plasmonic catalysis, astrophysics, materials science, and many other applications, molecules and materials are subject to high temperatures at which their electrons populate a wide distribution of energy levels. Nevertheless, most electronic structure methods to date have focused on the ground state, and those methods that do account for temperature either do not accurately account for electron correlation or have overwhelmingly been developed to study lattice models that do not capture the unique qualities of real materials. To rise to this challenge, the Rubenstein Group recently developed a new, fully ab initio, fully correlated finite temperature Auxiliary Field Quantum Monte Carlo (FT-AFQMC) method that proved to be able to yield exact results on a wide variety of benchmark molecules and simple solids. In this CAREER proposal, the Rubenstein Group aims to extend this technique to the study of heavier materials, including iron oxide, nickel oxide, vanadium oxide, and chromium triiodide, whose finite temperature electronic phase transitions have yet to be fully understood, while also developing a set of novel supporting mean field, selected CI (configuration interaction), and sampling techniques. These will not only improve FT-AFQMC’s performance, but can also serve as cheaper, stand-alone methods in their own right.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.

布朗大学的布伦达·鲁本斯坦（Brenda Rubenstein）由化学理论，模型和计算方法计划共同资助，以及刺激竞争研究（EPSCOR）的既定计划，以开发新方法，以建模相关材料的有限温度电子性能。在从催化到天体物理学再到材料科学的应用中，分子和材料可能会受到高温。然而，存在相对较少的理论来预测这些材料在这种温度下如何行为，从而挫败了我们设计材料（例如高-TC超导体和下一代热反应技术）的能力。作为该项目的一部分，Rubenstein组将开发一套互补的理论和仿真技术，这些理论和仿真技术将使在有限温度下进行复杂材料的高准确性建模。除这项研究外，Rubenstein Group将通过罗德岛美国化学学会项目和倡导计划（Rubenstein Dr. Rubenstein Leads）和Grant Arean高中学生的机会通过Brown University Ansive Seam Dements的真实实验，通过科学公平的计划，通过科学公平的过程来加强其持续的努力，以历史上的历史不足的高中学生在罗德岛州的高中学生进行积极的努力。 Rubenstein博士还正在开发一项新的加速化学发现课程和相关教科书，目的是通过如何利用数据科学来熟悉化学科学的本科生，以解决化学中的每日问题。该提案的核心目的是开发新的有限电子结构技术，以开发一系列新的有限的电子温度技术，以阐明电子相图材料的电子相图材料。在等离子体催化剂，天体物理学，材料科学以及许多其他应用中，分子和材料受到其电子的高温约束，其能量水平广泛。然而，迄今为止，大多数电子结构方法都集中在基态上，而那些确实说明温度的方法要么无法准确地说明电子相关性，要么已经开发出绝大多数来研究没有捕获真实材料独特品质的晶格模型。为了应对这一挑战，Rubenstein Group最近开发了一种全新的，完全相关的有限温度辅助磁场量子蒙特卡洛（FT-AFQMC）方法，该方法被证明能够在各种基准分子和简单固体上获得精确的结果。在这项职业建议中，Rubenstein Group旨在将该技术扩展到较重的材料的研究，包括氧化铁，氧化镍，氧化钒和三碘化物铬，其有限的温度电子相转换尚未充分理解，同时还需要开发一系列新颖的支撑域，选择了一组CI（配置）（配置）和Sampless技术。这些不仅可以提高FT-AFQMC的表现，而且可以作为其本身的廉价，独立的方法。该奖项反映了NSF的法定任务，并被认为是值得通过基金会的知识分子和更广泛影响的评估评估标准来通过评估来获得支持的。