Multiconfiguration Pair-Density Functional Theory for Complex Chemical Systems

复杂化学系统的多构型对密度泛函理论

• 批准号: 1764186
• 负责人: Laura Gagliardi
• 金额: $ 55万
• 依托单位: University of Minnesota-Twin Cities
• 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: 2018-08-01 至 2021-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1764186&HistoricalAwards=false
• 关键词: Multiconfiguration; Pair; Density; Functional; Theory

Laura Gagliardi and Donald G. Truhlar of the University of Minnesota are supported by an award from the Chemical Theory, Models and Computational Methods program in the Chemistry Division to develop a theory that enables high-accuracy calculations on chemical reactions on large systems. This method, Multi-Configuration Pair-Density Functional Theory (MC-PDFT), was recently introduced as a practical way to treat reactions where bonds are breaking, situations where electrons are excited, or systems that contain transition metals. All of these examples involve interactions among multiple electronic states, that are challenging problems for many other high accuracy methods in quantum chemistry. MC-PDFT is being broadly applied to systems in photochemistry, catalysis, supramolecular chemistry, and spectroscopy and thus has relevance in advanced manufacturing, renewable energy, and the chemical industry. In addition to the wide impact the method may have on the computational chemistry community, a broader impact of this proposal is the combination of expertise of two investigators, which allows students to benefit from a wider range of ideas and thereby contributes to well-rounded career preparation. Both investigators encourage women to enter scientific careers which contributes to a more diverse scientific workforce. Laura Gagliardi and Donald G. Truhlar are developing Multi-Configuration Pair-Density Functional Theory (MC-PDFT), a recent method for inherently multiconfigurational systems, that combines DFT with multiconfiguration wave functions. Their work is extending the theory in three directions. First, they are developing methods to calculate analytic gradients for state-averaged calculations, a feature that is important to enable exploration of excited states. Second, they are developing a state interaction method for treating multiple electronic states in regions near conical intersections. Third, they are incorporating MC-PDFT into additional software and are applying the methods to transition metal systems and excited states. One broader impact of this proposal is to combine the expertise of two investigators to allow students to benefit from a wide range of ideas, thereby contributing to well-rounded career preparation. Other important broader impacts stem from the technological importance of the research subjects chosen, especially for health, the material needs of society, industrial competitiveness, and defense.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.

明尼苏达大学的Laura Gagliardi和Donald G. Truhlar得到了化学理论，模型和计算方法计划的奖励，以开发一种理论，该理论能够对大型系统上的化学反应进行高准确的计算。 该方法是多种配置对密度密度理论（MC-PDFT），最近被引入是一种治疗键正在断裂的反应的实用方法，兴奋的电子或包含过渡金属的系统。 所有这些示例都涉及多个电子状态之间的相互作用，这对于量子化学中的许多其他高精度方法来说都是挑战性问题。 MC-PDFT广泛应用于光化学，催化，超分子化学和光谱法的系统，因此与先进的制造，可再生能源和化学工业具有相关性。 除了该方法对计算化学社区的广泛影响外，该提案的更广泛影响是两名研究人员的专业知识的结合，这使学生可以从更广泛的想法中受益，从而为全面的职业准备做出贡献。两位研究人员都鼓励妇女进入科学职业，这有助于更多样化的科学劳动力。 Laura Gagliardi和Donald G. truhlar正在开发多种配对密度函数理论（MC-PDFT），这是一种固有多种形式系统的最新方法，它将DFT与多构型波函数相结合。 他们的工作将理论扩展到三个方向。 首先，他们正在开发用于计算国家平均计算的分析梯度的方法，该功能对于实现激发态的特征很重要。 其次，他们正在开发一种状态相互作用方法，用于在圆锥形交集附近的区域中处理多个电子状态。 第三，他们将MC-PDFT纳入其他软件中，并将方法应用于过渡金属系统和激发态。该提案的一个更广泛的影响是结合两名研究人员的专业知识，以使学生能够从广泛的想法中受益，从而为全面的职业准备做出贡献。其他重要的更广泛的影响源于选择的研究对象的技术重要性，尤其是针对健康，社会的物质需求，工业竞争力和辩护。该奖项反映了NSF的法定任务，并被认为值得通过基金会的知识分子优点和更广泛的影响审查标准通过评估来进行评估。

项目成果

Multiconfiguration Pair-Density Functional Theory

• DOI: 10.1021/ct500483t
• 发表时间: 2014-09-01
• 期刊: JOURNAL OF CHEMICAL THEORY AND COMPUTATION
• 影响因子: 5.5
• 作者: Li Manni, Giovanni;Carlson, Rebecca K.;Gagliardi, Laura
• 通讯作者: Gagliardi, Laura

NWChem: Past, present, and future

NWChem：过去、现在和未来

• DOI: 10.1063/5.0004997
• 发表时间: 2020-05-14
• 期刊: JOURNAL OF CHEMICAL PHYSICS
• 影响因子: 4.4
• 作者: Apra, E.;Bylaska, E. J.;Harrison, R. J.
• 通讯作者: Harrison, R. J.

Scaling exchange and correlation in the on-top density functional of multiconfiguration pair-density functional theory: effect on electronic excitation energies and bond energies

• DOI: 10.1007/s00214-019-2539-6
• 发表时间: 2020-01
• 期刊: Theoretical Chemistry Accounts
• 影响因子: 1.7
• 作者: D. Presti;J. Kadlec;D. Truhlar;L. Gagliardi

M11plus, a Range-Separated Hybrid Meta Functional Incorporating Nonlocal Rung-3.5 Correlation, Exhibits Broad Accuracy on Diverse Databases

• DOI: 10.1021/acs.jpclett.0c00549
• 发表时间: 2020-04-16
• 期刊: JOURNAL OF PHYSICAL CHEMISTRY LETTERS
• 影响因子: 5.7
• 作者: Janesko, Benjamin G.;Verma, Pragya;Truhlar, Donald G.
• 通讯作者: Truhlar, Donald G.

Extended separated-pair approximation for transition metal potential energy curves

• DOI: 10.1063/5.0003048
• 发表时间: 2020-03-31
• 期刊: JOURNAL OF CHEMICAL PHYSICS
• 影响因子: 4.4
• 作者: Li, Shuhang J.;Gagliardi, Laura;Truhlar, Donald G.
• 通讯作者: Truhlar, Donald G.