Non-adiabatic quantum molecular dynamics of complex systems

复杂系统的非绝热量子分子动力学

• 批准号: 268264102
• 负责人: Dr. Ralph Welsch
• 金额: --
• 依托单位: Division of Chemistry and Chemical Engineering
• 依托单位国家: 德国
• 项目类别: Research Fellowships
• 财政年份: 2014
• 资助国家: 德国
• 起止时间: 2013-12-31 至 2015-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/268264102?language=en
• 关键词: Non; adiabatic; quantum; molecular; dynamics

Non-adiabatic transitions and quantum mechanical tunneling of protons are important processes in chemical and biochemical systems. The description of such processes in complex systems using non-adiabatic quantum dynamics methods is the aim of this project. In the last decade the ring-polymer molecular dynamics (RPMD) approach has shown to be a useful tool for approximate quantum dynamics simulations. Non-adiabatic processes cannot be described using the RPMD approach directly, but an extension of the RPMD approach to simulate two-state non-adiabatic processes, the kinetically constrained (KC) RPMD, was proposed very recently. The project aims to generalize and further develop the KC-RPMD approach. Furthermore, the approach will be used to investigate chemically and biochemically important non-adiabatic processes in complex systems. Several bioinorganic systems showing electron transfer processes (ET) or proton coupled electron transfer processes (PCET) can be considered: complexes based on Bis(imidazole) Iron Tetraphenylporphyrins, azurin proteins, a tris(phosphine)borane-supported iron complex, iron complexes with tris(phosphino)alkyl ligands featuring an axial carbon donor, cobalt complexes with diglyoxime ligands.

质子的非绝热跃迁和量子力学隧穿是化学和生物化学系统中的重要过程。这个项目的目的是用非绝热量子动力学方法描述复杂系统中的这种过程。在过去的十年中，环聚合物分子动力学（RPMD）方法已被证明是一个有用的工具，近似量子动力学模拟。非绝热过程不能直接用RPMD方法来描述，但RPMD方法的扩展来模拟两态非绝热过程，动力学约束（KC）RPMD，最近被提出。该项目旨在推广和进一步发展KC-RPMD方法。此外，该方法将用于研究复杂系统中化学和生物化学上重要的非绝热过程。可以考虑几种显示电子转移过程（ET）或质子耦合电子转移过程（PCET）的生物无机系统：基于双（咪唑）铁四苯基卟啉、天青蛋白、三（膦）硼烷支撑的铁络合物、具有轴向碳供体的三（膦基）烷基配体的铁络合物、具有丁二酮肟配体的钴络合物的络合物。

项目成果

Coherent two-dimensional terahertz-terahertz-Raman spectroscopy

• DOI: 10.1073/pnas.1605631113
• 发表时间: 2016-06-21
• 期刊: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• 影响因子: 11.1
• 作者: Finneran, Ian A.;Welsch, Ralph;Blake, Geoffrey A.
• 通讯作者: Blake, Geoffrey A.

Non-equilibrium dynamics from RPMD and CMD.

• DOI: 10.1063/1.4967958
• 发表时间: 2016-11
• 期刊: The Journal of chemical physics
• 作者: R. Welsch;Kai Song;Qiang Shi;S. Althorpe;Thomas F. Miller

Molecular Seesaw: How Increased Hydrogen Bonding Can Hinder Excited-State Proton Transfer.

• DOI: 10.1021/acs.jpclett.6b01391
• 发表时间: 2016-08
• 期刊: The journal of physical chemistry letters
• 作者: R. Welsch;E. Driscoll;J. Dawlaty;Thomas F. Miller