CAREER: Efficient and Reliable Electronic Structure Theories for Spectroscopic Properties of Strongly Correlated Systems

职业：强相关系统光谱特性的高效可靠的电子结构理论

• 批准号: 2044648
• 负责人: Alexander Sokolov
• 金额: $ 65万
• 依托单位: Ohio State University
• 依托单位国家: 美国
• 项目类别: Continuing 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=2044648&HistoricalAwards=false
• 关键词: CAREER; Efficient; Reliable; Electronic; Structure

Dr. Alexander Sokolov of the Ohio State University is supported by an award from the Chemical Theory, Models and Computational Methods (CTMC) program in the Division of Chemistry to develop theoretical methods that efficiently and accurately simulate spectroscopic properties of strongly correlated systems, such as conjugated organic molecules, transition metal compounds, and active sites of biological enzymes. Reliable simulations of how strongly correlated systems interact with light are crucial for understanding light-harvesting in photosynthesis, advancing technologies for solar energy conversion, and developing new photoactive materials with desired properties. However, available theoretical methods are unsatisfactory for simulating spectroscopic properties of strongly correlated systems due to limitations in their computational efficiency or accuracy. Dr. Sokolov and his group will fill this gap by developing a new framework of theoretical methods that combine efficient and accurate description of strongly correlated systems in many electronic states and provide access to a wide range of spectroscopic properties. All methods being developed by the Sokolov group will be implemented in a freely available and open-source computer program. The Sokolov group also develops hands-on, free, and publicly available computational lecture materials for use in undergraduate physical chemistry courses. Under this award, Dr. Sokolov will participate in local outreach activities to support middle school education in STEM (Science, Technology, Engineering and Mathematics) and increase public awareness of scientific research.With funding from the CTMC program, Dr. Sokolov and his team aim to develop robust, widely applicable, and computationally affordable multi-reference methods for simulations of spectroscopic properties of strongly correlated systems based on a framework of multireference algebraic diagrammatic construction theory. These new and systematically improvable methods have the potential to enable simulations of many (10’s or even 100’s) electronic transitions in a single computation, to allow for straightforward and efficient calculations of transition properties, and to be used to describe a variety of spectroscopic processes (e.g., optical or core excitations, two-photon absorption, etc.). More specifically, Dr. Sokolov and his group will work to develop new multi-reference methods for simulations of UV/Vis, near-edge X-ray absorption, and X-ray photoelectron spectra, as well as their efficient implementation for application to systems with a large number of strongly correlated orbitals and electrons. The Sokolov group research is integrated with an educational plan that aims (a) to strengthen undergraduate teaching of physical and computational quantum chemistry by developing hands-on computational lecture materials and designing a new computational chemistry course that incorporates training in scientific programming, and (b) to support middle school STEM education and public awareness of scientific research by participating in local outreach activities.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.

俄亥俄州立大学的Alexander Sokolov博士获得了化学学部化学理论、模型和计算方法（CTMC）项目的奖励，他开发了有效、准确地模拟强相关系统（如共轭有机分子、过渡金属化合物和生物酶活性位点）光谱特性的理论方法。对强相关系统如何与光相互作用的可靠模拟对于理解光合作用中的光收集、推进太阳能转换技术以及开发具有理想性能的新型光活性材料至关重要。然而，由于计算效率或精度的限制，现有的理论方法对强相关系统的光谱特性的模拟并不令人满意。Sokolov博士和他的团队将通过开发一种新的理论方法框架来填补这一空白，该框架结合了对许多电子状态下强相关系统的有效和准确描述，并提供了广泛的光谱特性。Sokolov小组开发的所有方法都将在一个免费的开源计算机程序中实现。Sokolov小组还开发了动手，免费和公开的计算讲座材料，用于本科物理化学课程。根据该奖项，Sokolov博士将参加当地的外展活动，以支持中学STEM（科学、技术、工程和数学）教育，并提高公众对科学研究的认识。在CTMC项目的资助下，Sokolov博士和他的团队旨在开发基于多参考代数图构造理论框架的强相关系统光谱特性模拟的强大的、广泛适用的、计算负担得起的多参考方法。这些新的系统改进的方法有可能在一次计算中模拟许多（10秒甚至100秒）电子跃迁，允许对跃迁性质进行直接有效的计算，并用于描述各种光谱过程（例如，光学或核心激发，双光子吸收等）。更具体地说，Sokolov博士和他的团队将致力于开发新的多参考方法，用于模拟UV/Vis，近边x射线吸收和x射线光电子能谱，以及它们在具有大量强相关轨道和电子的系统中的有效应用。Sokolov小组的研究与一项教育计划相结合，该计划旨在(a)通过开发动手计算讲座材料和设计包含科学规划培训的新计算化学课程来加强物理和计算量子化学的本科教学，以及(b)通过参与当地的外展活动来支持中学STEM教育和公众对科学研究的认识。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Simulating X-ray photoelectron spectra with strong electron correlation using multireference algebraic diagrammatic construction theory

• DOI: 10.1039/d1cp05476g
• 发表时间: 2022-01-27
• 期刊: PHYSICAL CHEMISTRY CHEMICAL PHYSICS
• 影响因子: 3.3
• 作者: de Moura, Carlos E., V;Sokolov, Alexander Yu
• 通讯作者: Sokolov, Alexander Yu

Quantifying and reducing spin contamination in algebraic diagrammatic construction theory of charged excitations

带电激发的代数图解构造理论中的量化和减少自旋污染

• DOI: 10.1063/5.0097333
• 发表时间: 2022
• 期刊: The Journal of Chemical Physics
• 作者: Stahl, Terrence L.;Banerjee, Samragni;Sokolov, Alexander Yu.
• 通讯作者: Sokolov, Alexander Yu.