Full quantum mechanical modeling of protonated water clusters

质子化水簇的全量子力学建模

• 批准号: 442507947
• 负责人: Professor Dr. Oriol Vendrell
• 金额: --
• 依托单位: Forschungsgruppe Theoretische Chemie
• 依托单位国家: 德国
• 项目类别: Research Grants
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/442507947?language=en
• 关键词: Full; quantum; mechanical; modeling; protonated

Over the past two years we have made very substantial progress towards the two main work packages set for the initial proposal: (1) automatic and on-the-fly determination of optimal tree structures in the context of the multi-layer multi-configurational time-dependent Hartree method; (2) full quantum mechanical modeling of the spectroscopy and dynamics of the extended Zundel (EZ) cation. The latter has been described in full dimensionality (51 D) using polyspherical coordinates and an exact kinetic energy operator, and on a very accurate neural-network potential energy surface provided by the group of Prof. D. Marx (U. Bochum). Specifically, we have developed and implemented tools for the automatic construction of wavefunction tensor trees, and we have been able to calculate good quality infrared spectra of the EZ system. The main aim of the extension project is still to push the boundaries for the full quantum dynamical description of flexible and highly correlated molecules and clusters through new methodological developments based on dynamical tensor-networks and the multi-configuration time-dependent Hartree Ansatz and to apply them to the full quantum mechanical description of the EZ cation in the gas phase and in solution. We have come a long way in the desired direction. In the extension period weplan to: (2.1) study in detail the connection between the Zundel and EZ spectra, and from this understand the microsolvation of the excess proton fully quantum-mecanically. (2.2) We plan to study the embedding of the EZ cation in external fields obtained from simulated environments, and thus take definite steps towards a full quantum characterization of the solvated proton in solution. Advancement in those areas will be important for the further understanding of solvated protons, protonated water clusters, and proton-relay networks fully quantum mechanically. Through the methodological developments of this project, we are pushing the state-of-the-art and enabling the full quantum simulation of large and flexible systems beyond current capabilities. Last but not least, all developments are being made immediately available to the community through the worldwide used Heidelberg MCTDH software package.

在过去的两年里，我们在为初始提案设定的两个主要工作包方面取得了非常实质性的进展：（1）在多层多配置时间相关的 Hartree 方法的背景下自动和即时确定最佳树结构； (2) 扩展 Zundel (EZ) 阳离子的光谱和动力学的全量子力学建模。后者已使用多球坐标和精确动能算子以及 D. Marx 教授（U. Bochum）小组提供的非常精确的神经网络势能表面进行全维（51 D）描述。 具体来说，我们开发并实现了自动构建波函数张量树的工具，并且我们已经能够计算出 EZ 系统的高质量红外光谱。该扩展项目的主要目标仍然是通过基于动态张量网络和多构型时间依赖性 Hartree Ansatz 的新方法论发展，突破柔性且高度相关的分子和团簇的完整量子动力学描述的界限，并将其应用于气相和溶液中 EZ 阳离子的完整量子力学描述。我们已经朝着期望的方向走了很长一段路。在延长期内，我们计划：（2.1）详细研究Zundel和EZ光谱之间的联系，并从中完全量子力学地理解过量质子的微溶剂化。 (2.2) 我们计划研究 EZ 阳离子在从模拟环境中获得的外部场中的嵌入，从而采取明确的步骤来对溶液中溶剂化质子进行全面的量子表征。这些领域的进步对于进一步理解溶剂化质子、质子化水簇和完全量子力学的质子中继网络非常重要。通过该项目的方法开发，我们正在推动最先进的技术，并使大型灵活系统的全面量子模拟超出当前的能力。最后但并非最不重要的一点是，所有开发成果都将通过全球使用的海德堡 MCTDH 软件包立即提供给社区。