CAREER: Photochemistry with Resonating Mean-Field

职业：光化学与共振平均场

• 批准号: 2236959
• 负责人: Shane Parker
• 金额: $ 65万
• 依托单位: Case Western Reserve University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-06-01 至 2028-05-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2236959&HistoricalAwards=false
• 关键词: CAREER; Photochemistry; Resonating; Mean; Field

With support from the Chemical Theory, Models, and Computational Methods (CTMC) program in the Division of Chemistry, Shane Parker of Case Western Reserve University will advance simulations of chemical reactions triggered by light. Chemical reactions that use or produce light are called photochemical reactions and are at the heart of many technologically and biologically important processes including photocatalysis, electricity generation in solar cells, and DNA damage caused by ultraviolet light. To reliably design new photocatalysts or photosensitizers, researchers need to understand the microscopic mechanism of photochemical reactions. Simulations based on quantum mechanics are a powerful tool for unraveling the mechanism of complicated photochemical reactions. However, the applicability of photochemistry simulations is limited by the quality of the available methods. Dr. Parker and his research group are developing the Resonating Mean-Field method for use in photochemistry simulations, thus enabling simulations with improved accuracy for classes of reactions that are inaccessible to current state-of-the-art methods. This project involves training and mentoring undergraduate and graduate students in theoretical chemistry and engagement with the Americal Chemical Society Project SEED to recruit high school students from Cleveland-area schools for summer research. In addition, Dr. Parker will build a suite of education-focused programs that run in web browsers so that K-12 students and university students can use numerical simulations to interrogate chemical models in the classroom.First-principles simulations have emerged as a powerful tool to discover the microscopic mechanism of complex photochemical reactivities at the heart of many important grand challenges for society, such as solar-fuel production on titanium dioxide nanoparticles. However, the use of such simulations for broad classes of problems is currently thwarted by the lack of affordable quantum chemistry methods that can balance the descriptions of electronic states with different charge and spin characteristics. To address this need, Dr. Parker and his research group are developing the Resonating Mean-Field (ResMF) method for photochemistry simulations. ResMF is a promising method for photochemistry simulations because it has a mean-field cost, explicitly balances states with different characters and reproduces the correct topology of conical intersections. The research objectives of this proposal are i) to establish a nonorthogonal spin-adapted wavefunction expansion that eliminates spin-contamination and reduces computational cost, ii) to produce a numerically robust and efficient implementation of ResMF, and iii) to implement all molecular forces and properties necessary to simulate photochemistry. The educational objectives of this proposal are i) to develop web-based numerical simulation tools for use in classrooms of all levels, ii) to train K-12 educators to teach model-based thinking skills, and iii) to introduce high school students from Cleveland-area schools to scientific research.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.

在化学理论，模型和计算方法（CTMC）方案的支持下，Case Western Reserve University的Shane Parker将推动对光触发的化学反应的模拟。使用或产生光的化学反应称为光化学反应，是许多技术和生物学上重要的过程的核心，包括光催化，太阳能电池中的发电以及由紫外线引起的DNA损伤。为了可靠地设计新的光催化剂或光敏剂，研究人员需要了解光化学反应的微观机制。基于量子力学的仿真是阐明复杂光化学反应机制的强大工具。但是，光化学模拟的适用性受可用方法质量的限制。 Parker博士及其研究小组正在开发用于光化学模拟的共鸣均值方法，从而为当前最新方法无法访问的反应提供了提高准确性的模拟。该项目涉及培训和指导学者化学的本科生和研究生，并与Americal Chemical Society Project Seed进行参与，以招募来自克利夫兰地区学校的高中生进行夏季研究。 此外，帕克博士还将建立一套以教育为中心的计划，以在网络浏览器中运行，以便K-12学生和大学生可以使用数值模拟在课堂上询问化学模型。首先出现了一种强大的工具，可以作为一种在许多重要的策略中，例如，在许多重要的光化机制中，例如，在许多重要的社会中发现了诸如Society的综合挑战，例如Society-Fuelar for Society，例如纳米颗粒。但是，由于缺乏负担得起的量子化学方法，可以平衡具有不同电荷和自旋特性的电子状态的描述，因此目前将这种模拟用于广泛的问题。为了满足这一需求，帕克博士和他的研究小组正在开发用于光化学模拟的共鸣均值（RESMF）方法。 RESMF是光化学模拟的一种有前途的方法，因为它具有平均场地成本，明确平衡状态与不同的特征，并重现了锥形交叉点的正确拓扑。该提案的研究目标是i）建立一个非正交旋转适应的波函数扩展，从而消除了自旋 - 污染和降低计算成本，ii）生成了RISMF的数值和高效实现，以及III），以实现所有分子力和实施所需的所有分子力和属性，以模拟光学的光学精确性。该提案的教育目标是i）开发基于网络的数值模拟工具，用于在各个级别的教室中使用，ii）培训K-12教育者教授基于模型的思维技能，以及iii），以介绍克利夫兰地区学校的高中学生，向科学研究进行科学研究。这项奖项反映了NSF的法定任务，反映了通过评估的范围的范围，这是一项范围的构成者的范围。