Exploring potential energy surfaces for strong field chemistry, ion dynamics and bio-organic chemistry

探索强场化学、离子动力学和生物有机化学的势能面

• 批准号: 1212281
• 负责人: Hans Schlegel
• 金额: $ 46万
• 依托单位: Wayne State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2012
• 资助国家: 美国
• 起止时间: 2012-08-01 至 2015-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1212281&HistoricalAwards=false
• 关键词: Exploring; potential; energy; surfaces; strong

H. Bernhard Schlegel of Wayne State University is supported by an award from the Chemical Theory, Models and Computational Methods program in the Chemistry Division to explore projects in strong field chemistry, ab initio molecular dynamics, bio-organic systems, and reaction path optimization. Explicitly, integration of time dependent configuration interaction (TD-CI) and density functional theory will be compared for modeling molecules interacting with short, intense laser pulses. Different methods for simulating strong field ionization will be assessed. TD-CI simulations with field-dependent states and improved methods for integrating ab initio classical trajectories in strong fields will be developed. Standard and long-range corrected functionals will be compared for classical trajectories in strong laser fields. These ab initio molecular dynamics methods will be used to study the kinetic energy distribution of protons in strong field fragmentations, and H(+) migration and H3(+) formation from molecules interacting with intense laser fields. Studies of bio-organic systems will include redox potentials of intermediates in guanine oxidation pathways, environmental effects on nucleobase pKa's and redox potentials, guanine-thymine crosslinks and metal-promoted oxidation of guanine. To support these studies, new methods will be developed for reaction path optimization, reaction paths through seams and conical intersections, and reaction paths for bifurcating potential energy surfaces.Understanding molecular dynamics and exploring reaction pathways are key challenges in chemistry. Strong field chemistry and attosecond science address these challenges by using short intense laser pulses to probe structure and reactivity. Professor Schlegel and his team are developing new methods for simulating the behavior of molecules under these extreme conditions. The selected studies of bio-organic systems include properties and reactivity of DNA bases related to toxicity, mutagenesis and cancer. To support these studies, the researchers are developing new methods for exploring reaction paths on potential energy surfaces that will benefit many areas of chemistry which utilize molecular orbital calculations.

韦恩州立大学的H·伯恩哈德·施莱格尔得到了化学部化学理论、模型和计算方法项目的支持，该奖项旨在探索强场化学、从头算分子动力学、生物有机系统和反应路径优化等项目。显然，我们将比较含时组态相互作用(TD-CI)和密度泛函理论的集成，以模拟分子与短而强的激光脉冲的相互作用。我们将评估模拟强场电离的不同方法。将开发依赖于场的TD-CI模拟和改进的方法来积分强场中的从头算经典轨迹。我们将比较标准和长程修正泛函在强激光场中的经典轨迹。这些从头算分子动力学方法将被用来研究质子在强场碎裂中的动能分布，以及分子与强激光相互作用时H(+)的迁移和H3(+)的形成。生物有机系统的研究将包括鸟嘌呤氧化途径中中间体的氧化还原电位、环境对核苷酸碱基PKA和氧化还原电位的影响、鸟嘌呤-胸腺嘧啶交联物以及金属促进的鸟嘌呤氧化。为了支持这些研究，将开发新的方法来优化反应路径，通过接缝和锥形相交的反应路径，以及分叉势能面的反应路径。了解分子动力学和探索反应路径是化学中的关键挑战。强场化学和阿秒科学通过使用短而强的激光脉冲来探测结构和反应性来应对这些挑战。施莱格尔教授和他的团队正在开发新的方法来模拟分子在这些极端条件下的行为。选定的生物有机系统研究包括与毒性、突变和癌症相关的DNA碱基的性质和反应能力。为了支持这些研究，研究人员正在开发新的方法来探索势能面上的反应路径，这将使利用分子轨道计算的许多化学领域受益。