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.

Laura Gagliardi和Donald G.明尼苏达大学的Truhlar得到了化学系化学理论，模型和计算方法项目的支持，以开发一种能够对大型系统的化学反应进行高精度计算的理论。 这种方法，多组态对密度泛函理论（MC-PDFT），最近被引入作为一种实用的方法来处理键断裂的反应，电子被激发的情况下，或包含过渡金属的系统。 所有这些例子都涉及多个电子态之间的相互作用，这对于量子化学中的许多其他高精度方法来说是具有挑战性的问题。 MC-PDFT被广泛应用于光化学、催化、超分子化学和光谱学系统，因此在先进制造、可再生能源和化学工业中具有相关性。 除了该方法可能对计算化学界产生的广泛影响外，该提案的更广泛影响是两名研究人员的专业知识相结合，这使学生能够从更广泛的想法中受益，从而有助于全面的职业准备。两位研究人员都鼓励妇女从事科学工作，这有助于建立更加多样化的科学工作队伍。 Laura Gagliardi和Donald G. Truhlar正在开发多组态对密度泛函理论（MC-PDFT），这是一种将DFT与多组态波函数相结合的固有多组态系统的最新方法。 他们的工作是在三个方向上扩展这一理论。 首先，他们正在开发用于计算状态平均计算的分析梯度的方法，这一特征对于探索激发态非常重要。 其次，他们正在开发一种状态相互作用方法，用于处理圆锥形交叉点附近区域的多个电子状态。 第三，他们正在将MC-PDFT整合到其他软件中，并将这些方法应用于过渡金属系统和激发态。这一提议的一个更广泛的影响是将两名调查员的专业知识联合收割机结合起来，让学生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所选择的研究课题的技术重要性，特别是对健康，社会的物质需求，工业竞争力和国防。该奖项反映了NSF的法定使命，并已被认为是值得通过使用基金会的智力价值和更广泛的影响审查标准进行评估的支持。

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

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

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.

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.

Multi-state pair-density functional theory

• DOI: 10.1039/d0fd00037j
• 发表时间: 2020-12-01
• 期刊: FARADAY DISCUSSIONS
• 影响因子: 3.4
• 作者: Bao, Jie J.;Zhou, Chen;Truhlar, Donald G.
• 通讯作者: Truhlar, Donald G.