Density Functional Theory of Electronic Structure

电子结构密度泛函理论

• 批准号: 2344734
• 负责人: John Perdew
• 金额: $ 42万
• 依托单位: Tulane University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2024
• 资助国家: 美国
• 起止时间: 2024-02-01 至 2024-10-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2344734&HistoricalAwards=false
• 关键词: Density; Functional; Theory; Electronic; Structure

NONTECHNICAL SUMMARYThe Division of Materials Research and the Division of Chemistry contribute funds to this award that supports theoretical research, computation, and education to develop more accurate computer modeling of molecules, chemicals, and materials. To do this, the PI will focus on the “glue” that binds one atom to another to form molecules and materials: the exchange-correlation energy. In this research, the PI will develop even more accurate approximations for this “glue” that still permit efficient simulation on computers.Kohn-Sham density functional theory is widely used in physics, chemistry, and materials science to predict what atoms, molecules, and materials can exist and with what properties. Starting from the first principles of quantum mechanics, this theory constructs the ground-state energy and electron density of a many-electron system from an auxiliary system of non-interacting electrons including the contribution from the "glue", facilitating practical computation. The exact exchange-correlation energy must be approximated. Widely predictive approximations should themselves be based upon first principles, and be accurate enough to predict the small energy differences between competing states in complex materials and systems. The strategy of this project is to achieve more accurate but computable general-purpose approximations by incorporating more of the mathematical properties of the exact universal density functional for the exchange-correlation energy, i.e., by satisfying more exact constraints, by fitting to more appropriate systems in which the approximation can be either exact or highly accurate, and by carefully testing and validating the new approximations over a wide range of systems. Long-term practical benefits to society could include new medicines, chemicals, materials or devices. This research program educates graduate students and more advanced researchers as developers, validators, and users of density functional and electronic structure theory. It will furthermore engage undergraduates and high-school students in the excitement of scientific discovery. The PI will also work with TUteach students and administrators along with other interested individuals in Temple Physics, to organize an annual High School Physics Day at Temple which would be focused on invited high school physics teachers.TECHNICAL SUMMARYThe Division of Materials Research and the Division of Chemistry contribute funds to this award that supports theoretical research, computation, and education to develop more accurate and predictive density functionals for the exchange-correlation energy, while retaining the advantage of relative computational efficiency. These functionals will be designed to satisfy the known exact constraints on the exact functional. A smoother and more perfected version of the SCAN (strongly constrained and appropriately normed) meta-generalized gradient approximation will be developed, using as appropriate norms not only the uniform electron gas but also many real atoms. Also, the PI aims to continue developing a generalized Perdew-Zunger self-interaction correction to the improved SCAN that should be exact for all one-electron densities without losing accuracy for many-electron densities. These advanced functionals will be tested on the many systems for which SCAN has succeeded, including liquid water, structural energy differences in solids, artificial molecules, and the high-temperature superconducting materials, and on the few for which it is known to fail, such as some bulk transition metals and alloys, as well as on additional complex or strongly-correlated systems. Improvements to long-range van der Waals corrections, and a self-interaction correction to the random phase approximation, will also be made and validated. Understanding what makes a functional predictive should guide the burgeoning effort to develop density functional approximations by machine learning. The intellectual merit of the proposal is that many known mathematical properties of the exact functional should make the resulting approximate functionals widely and accurately predictive, at reasonable computational cost, and thus make them useful for many applications, not only for the simpler molecules and materials for which density functionals are already reliable, but also for the more complex or strongly-correlated ones. In particular improved functionals are critically needed for high-throughput searches for new materials with desired properties. The small energy differences between different states can make a complex material easy to switch under human control from one state and functionality to another.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.

非技术总结材料研究和化学划分为该奖项提供了资金，该奖项支持理论研究，计算和教育，以开发分子，化学品和材料的更准确的计算机建模。为此，PI将集中于将一个原子与另一个原子结合以形成分子和材料的“胶水”：交换相关能量。在这项研究中，PI将为这种“胶水”开发更准确的近似值，该“胶水”仍然可以在计算机上有效模拟。Kohn-Sham密度功能理论被广泛用于物理，化学和材料科学，以预测可以存在的原子，分子和材料可以存在的以及具有什么特性。从量子力学的第一原理开始，该理论从非相互作用电子的辅助系统中构建了许多电子系统的基础能量和电子密度，包括“胶水”的贡献，支持实践计算。必须近似确切的交换相关能。广泛的预测性近似值本身应基于第一原理，并且足够准确，以预测复杂材料和系统中竞争状态之间的较小能量差异。该项目的策略是通过合并更多的通用密度的数学特性来实现更准确但可计算的通用近似值，以实现交换可相关能量的功能，即，通过满足更确切的系统来满足更合适的系统，在这些系统中可以通过这些系统进行精确或高度准确或高度准确的测试，并仔细地测试和效率范围范围范围，并且要仔细测试和有效的范围。对社会的长期实际利益可能包括新药物，化学药品，材料或设备。该研究计划将研究生和更高级的研究人员作为开发人员，验证者以及密度功能和电子结构理论的使用者进行教育。它将进一步吸引本科生和高中生的科学发现兴奋。 PI还将与Tuteach的学生和管理人员以及寺庙物理学中的其他有趣的人一起在神庙中组织一个年度高中物理日，该日将集中在受邀的高中物理教师上。技术总结材料研究和化学部的划分，化学划分为这项奖项提供了贡献的资金，以支持更多的精确研究，以发展精确的研究，以开发精确的计算，以开发出来的计算，并具有限制性的范围。 效率。这些功能将设计为满足确切功能的已知确切约束。将开发扫描的平滑，更完美的版本（严格约束且适当地归一化）荟萃化梯度近似，不仅是适当的规范，不仅是均匀的电子气体，而且还使用许多真实原子。此外，PI旨在继续开发一般的Perdew-Zunger自我交织校正，以改进的扫描，这对于所有一单电子密度而言应该是确切的，而不会因多种电子密度而失去准确性。这些高级功能将在许多系统上进行测试，以改进远程范德华校正，并且还将对随机相位近似进行自我相互作用校正。了解什么使功能性预测性应指导通过机器学习来开发密度功能近似的新兴努力。该提案的智力优点在于，确切功能的许多已知数学特性应使所得的近似函数范围广，准确地预测性，以合理的计算成本，从而使它们对许多应用程序有用，而不仅仅是对更简单的分子和材料的较简单的密度和材料，那么它已经是可靠的，而且对更复杂或强烈的或强的或强的函数也是如此。对于具有所需特性的新材料的高通量搜索，特别需要改进的功能。不同国家之间的较小能量差异可以使复杂的材料易于在人类控制下从一个州和功能转换为另一种状态。该奖项反映了NSF的法定任务，并且使用基金会的知识分子优点和更广泛的影响审查标准，被认为是值得通过评估的。

项目成果

Incorporation of density scaling constraint in density functional design via contrastive representation learning

• DOI: 10.1039/d3dd00114h
• 发表时间: 2022-05
• 期刊: Digital Discovery
• 作者: Weiyi Gong;Tao Sun;Hexin Bai;S. Chowdhury;Peng Chu;Anoj Aryal;Jie Yu;H. Ling;J. Perdew;Q. Yan

Comparing first-principles density functionals plus corrections for the lattice dynamics of YBa2Cu3O6

比较 YBa2Cu3O6 晶格动力学的第一原理密度泛函和修正

• DOI: 10.1063/5.0181349
• 发表时间: 2024
• 期刊: The Journal of Chemical Physics
• 作者: Ning, Jinliang;Lane, Christopher;Barbiellini, Bernardo;Markiewicz, Robert S.;Bansil, Arun;Ruzsinszky, Adrienn;Perdew, John P.;Sun, Jianwei
• 通讯作者: Sun, Jianwei

Unconventional Error Cancellation Explains the Success of Hartree–Fock Density Functional Theory for Barrier Heights

非常规误差消除解释了 Hartree-Fock 势垒高度密度泛函理论的成功

• DOI: 10.1021/acs.jpclett.3c03088
• 发表时间: 2024
• 期刊: The Journal of Physical Chemistry Letters
• 作者: Kanungo, Bikash;Kaplan, Aaron D.;Shahi, Chandra;Gavini, Vikram;Perdew, John P.
• 通讯作者: Perdew, John P.

The Predictive Power of Exact Constraints and Appropriate Norms in Density Functional Theory

密度泛函理论中精确约束和适当规范的预测能力

• DOI: 10.1146/annurev-physchem-062422-013259
• 发表时间: 2023
• 期刊: Annual Review of Physical Chemistry
• 影响因子: 14.7
• 作者: Kaplan, Aaron D.;Levy, Mel;Perdew, John P.
• 通讯作者: Perdew, John P.

Challenges for density functional theory in simulating metal–metal singlet bonding: A case study of dimerized VO2

密度泛函理论在模拟金属-金属单线态键合中面临的挑战：二聚 VO2 的案例研究

• DOI: 10.1063/5.0180315
• 发表时间: 2024
• 期刊: The Journal of Chemical Physics
• 作者: Zhang, Yubo;Ke, Da;Wu, Junxiong;Zhang, Chutong;Hou, Lin;Lin, Baichen;Chen, Zuhuang;Perdew, John P.;Sun, Jianwei
• 通讯作者: Sun, Jianwei