Fluctuation-Based Electronic Structure Methods

基于涨落的电子结构方法

• 批准号: 1800431
• 负责人: Filipp Furche
• 金额: $ 49万
• 依托单位: University of California-Irvine
• 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: 2018-04-15 至 2021-03-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1800431&HistoricalAwards=false
• 关键词: Fluctuation; Based; Electronic; Structure; Methods

Filipp Furche of the University of California, Irvine is supported by an award from the Chemical Theory, Models and Computational Methods Program in the Division of Chemistry to develop, implement, test, and apply novel computational chemistry methods. The Condensed Matter and Materials Theory program in the Division of Materials Research also contributes to this award. The new methods enable simulations of molecules and condensed matter systems that are very difficult to treat with conventional approaches, for example rare-earth compounds or transition metal compounds used in catalysis. Such systems are critically importance for science and emerging technologies. A fundamentally different approach to electronic structure theory based on quantum fluctuations, proposed by Furche promises to overcome many of these limitations. The methods developed in this project are made available to the public through the Turbomole quantum chemistry software. The project enhances undergraduate education and workforce readiness through a new concentration in Theoretical and Computational Chemistry at UCI and a high school outreach program aimed at students from disadvantaged backgrounds.Furche and his group are developing new methodology to enable predictive simulations of molecules and condensed matter systems such as small-bandgap or correlated materials and clusters, noncovalently bound nanostructures, or optical properties of transition-metal and rare earth compounds. Despite their critical importance for science and emerging technologies, these systems remain nearly intractable with conventional electronic structure methods, due to insufficient accuracy, computational efficiency, or both. Random phase approximation (RPA) methods developed during previous funding periods are the prototype fluctuation-based electronic structure theory. Guided by the successes and failures of RPA, Furche and his group are laying the groundwork for a systematically improvable hierarchy of electronic structure methods based on fluctuations. As opposed to the conventional approach to electron correlation in chemistry, which is based on interacting electron pairs, triples, etc., the methods proposed here describe correlation in many-electron systems by vacuum fluctuations generated by virtual pairs of electrons and holes traveling forward and backward in time (and multiples thereof). Furche and his group also explore a Brueckner functional framework as alternative to Kohn-Sham reference states, and aim to extend the scope of RPA methods to ionization, time-dependent properties, and excited states. Applications include low-valent rare-earth and actinide compounds, and halogen-pi interaction mediated drug design.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.

加州大学欧文分校的Filipp Furche由化学部化学理论、模型和计算方法计划颁发的奖项支持，以开发、实施、测试和应用新的计算化学方法。材料研究部的凝聚态物质和材料理论项目也为这一奖项做出了贡献。这些新方法可以模拟分子和凝聚态物质体系，这些分子和凝聚态物质体系很难用传统方法处理，例如用于催化的稀土化合物或过渡金属化合物。这样的系统对科学和新兴技术至关重要。Furche提出了一种基于量子涨落的完全不同的电子结构理论方法，有望克服其中的许多局限性。在这个项目中开发的方法通过透波莫尔量子化学软件向公众开放。该项目通过UCI理论和计算化学的新集中以及针对弱势背景学生的高中推广计划，提高了本科教育和劳动力准备。Furche和他的团队正在开发新的方法，以实现对分子和凝聚态系统的预测模拟，如小带隙或相关材料和团簇、非共价束缚纳米结构，或过渡金属和稀土化合物的光学性质。尽管它们对科学和新兴技术至关重要，但由于精度和/或计算效率的不足，这些系统仍然几乎无法用传统的电子结构方法解决。随机相位近似(RPA)方法是基于涨落的电子结构理论的原型。在RPA的成功和失败的指导下，Furche和他的团队正在为基于涨落的电子结构方法的系统改进层次奠定基础。与化学中基于相互作用的电子对、三重态等的传统电子关联方法不同，这里提出的方法描述了多电子系统中由虚拟电子对和空穴在时间上向前和向后移动(及其倍数)所产生的真空涨落的关联。Furche和他的团队还探索了Brueckner泛函框架作为Kohn-Sham参考态的替代，并旨在将RPA方法的范围扩展到电离、依赖于时间的性质和激发态。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势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

Effect of Ammonium Salts on the Decarboxylation of Oxaloacetic Acid in Atmospheric Particles

铵盐对大气颗粒物中草酰乙酸脱羧的影响

• DOI: 10.1021/acsearthspacechem.1c00025
• 发表时间: 2021
• 期刊: ACS Earth and Space Chemistry
• 影响因子: 3.4
• 作者: Klodt, Alexandra L.;Zhang, Kimberly;Olsen, Michael W.;Fernandez, Jorge L.;Furche, Filipp;Nizkorodov, Sergey A.
• 通讯作者: Nizkorodov, Sergey A.

Synthesis and Magnetism of Neutral, Linear Metallocene Complexes of Terbium(II) and Dysprosium(II)

• DOI: 10.1021/jacs.9b05816
• 发表时间: 2019-08-21
• 期刊: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
• 影响因子: 15
• 作者: Gould, Colin A.;McClain, K. Randall;Long, Jeffrey R.
• 通讯作者: Long, Jeffrey R.

Variational generalized Kohn-Sham approach combining the random-phase-approximation and Green's-function methods

• DOI: 10.1103/physreva.99.012518
• 发表时间: 2019-01
• 期刊: Physical Review A
• 影响因子: 2.9
• 作者: Vamsee K. Voora;S. Balasubramani;F. Furche

Selfconsistent random phase approximation methods

自洽随机相位逼近方法

• DOI: 10.1063/5.0056565
• 发表时间: 2021
• 期刊: The Journal of Chemical Physics
• 作者: Yu, Jason M.;Nguyen, Brian D.;Tsai, Jeffrey;Hernandez, Devin J.;Furche, Filipp
• 通讯作者: Furche, Filipp

Tertiary Alcohols as Radical Precursors for the Introduction of Tertiary Substituents into Heteroarenes

• DOI: 10.1021/acscatal.9b00405
• 发表时间: 2019-03
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: S. P. Pitre;Mikko Muuronen;D. Fishman;L. Overman