MOLECULAR DYNAMICS STUDY ON REAGENT DENSITY DEPENDENCE AND TEMPERATURE-PRESSURE EFFECT IN SOLUTION CHEMICAL REACTIONS

溶液化学反应中试剂密度依赖性和温压效应的分子动力学研究

• 批准号: 13440176
• 负责人: NAGAOKA Masataka
• 金额: $ 0.58万
• 依托单位: NAGOYA UNIVERSITY
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (B)
• 财政年份: 2001
• 资助国家: 日本
• 起止时间: 2001 至 2002
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-13440176/
• 关键词: FREE-ENERGY GRADIENT METHOD; QM; MM-MD METHOD; FREE-ENERGY PERTURBATION; FREE-ENERGY SURFACE; MOLECULAR DYNAMICS; MICRO-ENTROPY EFFECT; STRUCTURE OPTIMIZATION; TEMPERATURE-PRESSURE EFFECT; ハイブリッドQM; 分子軌道法; メンシュトキン反応; 微視的エントロピー; 自由エネルギー面; 遷移状

(1) Combining Monte Carlo method, Molecular Dynamics method and the statistical perturbation method, the force fields on the free energy hypersurface were calculated for several interesting chemically reacting systems in solution.(2) The numerical algorythm of stochastic partial differential equation that the head investigator completed in 2001, was coded to develop a program to solve a simultaneous equations of motion for a quantum-classical mixed reacting system.(3) We have clarified the microscopic reaction dynamics in solution, especially for Menshutkin reaction, and explained some typical characteristics by calculating the free energy profile along the intrinsic reaction coordinate, which was executed by the free energy gradient method.(4) At the end of the research term, several results with respect to the free energy profiles for several chemical reactions in solution, were published in a few important meetings, e.g., the annual meetings of Japan Chemical Society. Further, they were collected and published as several research articles as described in the following section, i.e., 11 REFERENCE.

(1) 结合蒙特卡罗方法、分子动力学方法和统计摄动方法，计算了溶液中几种有趣的化学反应体系的自由能超曲面上的力场。(2) 随机偏微分方程的数值算法研究者于 2001 年完成，被编码开发一个程序来求解量子经典混合反应系统的联立运动方程。(3) 我们已经阐明了微观反应动力学解决方案，特别是 Menshutkin 反应，并通过计算沿着本征反应坐标的自由能分布来解释一些典型特征，这是通过自由能梯度方法执行的。（4）在研究期结束时，关于溶液中几种化学反应的自由能曲线在一些重要会议上发表，例如日本化学会年会。此外，它们被收集并作为几篇研究文章发表，如以下部分（即 11 参考文献）所述。

项目成果

Yoichi Yamaguchi, et al.: "Theoretical Prediction of Proton Chemical Shift in Supercritical Water using Gas-phase Approximation"Chem. Phys. Lett.. 348. 129-136 (2001)

Yoichi Yamaguchi 等人：“使用气相近似对超临界水中质子化学位移的理论预测”Chem。

Masataka Nagaoka, et al.: "Advances in Quantum Monte Carlo Method"World Scientific. (2002)

Masataka Nagaoka 等人：“量子蒙特卡罗方法的进展”世界科学。

Hajime Hirao, et al.: "Transition-state Optimization by the Free Energy Gradient Method : Application to Aqueous-phase Menshutkin Reaction between Ammonia and Methyl Chloride"Chem. Phys. Lett.. 348. 350-356 (2001)

Hajime Hirao 等人：“通过自由能梯度法进行过渡态优化：在氨和氯甲烷之间的水相 Menshutkin 反应中的应用”Chem。

M.Nagaoka, et al.: "Toward Quantum Chemodynamics in Condensed Phase via Stochastic Quantization Method"Recent Advances in Quantum Monte Calro Methods II. 254-278 (2002)

M.Nagaoka 等人：“通过随机量化方法实现凝聚相中的量子化学动力学”量子蒙特卡罗方法的最新进展 II。

M.Nagaoka, et al.: "Structure Optimization by the Free Energy Gradient Method II Illustration by Ammonia-Water Molecule Pair in Aqueous Solution"Journal of Chemical Physics. (投稿中).

M.Nagaoka 等人：“通过自由能梯度方法 II 说明水溶液中的氨-水分子对进行结构优化”化学物理杂志（进行中）。