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CAREER: Investigation of Laser-driven Chemical Reactions by Molecular Dynamics

职业：通过分子动力学研究激光驱动的化学反应

基本信息

批准号：
1944921
负责人：
Dmitri Kilin
金额：
$ 65万
依托单位：
North Dakota State University Fargo
依托单位国家：
美国
项目类别：
Continuing Grant
财政年份：
2020
资助国家：
美国
起止时间：
2020-08-01 至 2025-07-31
项目状态：
未结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1944921&HistoricalAwards=false
关键词：
CAREER Investigation Laser driven Chemical

项目摘要

Dmitri Kilin of North Dakota State University is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry for theoretical research focused on the control of chemical reactions driven by light, called photoreactions. Light can activate, direct, and speed up chemical reactions otherwise inaccessible by conventional reaction conditions like heat. The goal of this research is to study and simulate the control of photochemical reactions through the tuning of specialized laser light. These researchers develop distributable software with which users can explore light-driven chemical reactions. The software will help advance a wide range of technologies, including energy conversion and storage, and chemical sensing. This work will contribute to theory-guided optimization of thin-film deposition technology, which is important for the miniaturization of electronic circuits towards nano- and sub-nano scales. The educational mission includes the participation of graduate and undergraduate students in professional activities. Outreach activities are focused on providing to tribal college students at Native American reservations research experience via participations in the Nurturing American Tribal Undergraduate Research and Education (NATURE) Program at NDSU, which will specifically benefit from remote/distant learning/training/research opportunities. Dr. Kilin will also mentor high school students participating in PICNICS (Parents Involvement with Children, Nurturing Intellectual Curiosity in Science) program hosted at NDSU.The computational description of dynamics under the electromagnetic field remains challenging due to coupled electronic and nuclear degrees of freedom. There are known approaches for independent treatment of subsequent contributing processes: photoexcitation, reorganization and dissipative interaction with electronic degrees of freedom, and molecular and reaction dynamics of nuclear degrees of freedom. However, on a short timescale, all three are coupled. The Kilin group is developing first-principles molecular dynamics approaches for coupled electrons, nuclei, and light to fill the gap in computational investigation of laser-driven chemical reactions. The approaches rely on the combination of Rabi theory and surface hopping approximations. The research program includes an effort for validation of utilized approximations. A hypothesis driven search of acceptable approximations showing accuracy versus numerical cost facilitates an effort of establishing standard approaches for reactions at extreme conditions. Various corrections are being implemented accounting for the quantization of nuclear degrees of freedom, the higher level of electronic structure calculations with increased precision, and the treatment of coherent superposition of quantized states. The practical applications of the improved methodologies focus on photofragmentation of metal-organic compounds, photopolymerization of silicon containing compounds, photografting, and photodesorption of covalent functional groups on carbon nanotubes. The theoretical tools being developed can be applicable to interpret and predict reaction mechanisms and distribution of products for various classes of reactions.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.

北达科他州州立大学的德米特里·基林获得了化学系化学理论、模型和计算方法项目的支持，以表彰其专注于控制光驱动的化学反应，即光反应的理论研究。光可以激活、引导和加速化学反应，否则传统的反应条件如热是无法达到的。本研究的目的是研究和模拟通过特殊的激光调谐来控制光化学反应。这些研究人员开发了可分发的软件，用户可以使用该软件来探索光驱动的化学反应。该软件将有助于推进广泛的技术，包括能源转换和存储，以及化学传感。这项工作将有助于理论指导薄膜沉积技术的优化，这对于电子电路向纳米和亚纳米尺度的小型化具有重要意义。教育使命包括研究生和本科生参与专业活动。外展活动的重点是通过参加南加州州立大学的培育美国部落本科生研究和教育(自然)方案，向美洲原住民保留地的部落大学生提供研究经验，该方案将特别受益于远程学习/培训/研究机会。Klin博士还将指导参加NDSU举办的野餐(父母与孩子的参与，在科学中培养智力好奇心)项目的高中生。由于电子和核自由度的耦合，电磁场下的动力学的计算描述仍然具有挑战性。已知有独立处理后续贡献过程的方法：具有电子自由度的光激发、重组和耗散相互作用，以及核自由度的分子和反应动力学。然而，在很短的时间范围内，这三个因素都是相互关联的。科林小组正在为耦合电子、原子核和光开发第一原理分子动力学方法，以填补激光驱动化学反应计算研究的空白。这些方法依赖于Rabi理论和表面跳跃近似的结合。该研究计划包括对所使用的近似进行验证的努力。假设驱动的对可接受的近似的搜索显示了准确性与数值成本的关系，这有助于为极端条件下的反应建立标准方法。考虑到核自由度的量子化、更高水平的电子结构计算提高了精度以及量子化态的相干叠加的处理，正在进行各种修正。这些改进方法的实际应用主要集中在金属有机化合物的光裂解、含硅化合物的光聚合、光接枝以及碳纳米管上共价官能团的光解吸等方面。正在开发的理论工具可以应用于解释和预测各类反应的反应机理和产品分布。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。