报告题目（Title）：从头计算法分子动力学模拟复杂溶液系统（Ab-initio Simulations of CondensedAqueous Systems）
报告人（Speaker）：Dr. Jinggang Lan (UZH - Universität Zürich)
报告地点（Place）：腾讯会议（ID: 562 734 343）
Condensed aqueous systems serve an important role in many scientific fields such as materials science, electro- chemistry and nanotechnology. Many important reactions occur in aqueous phases or at aqueous solid interfaces. Understanding these processes may provide useful insights on improving the reactivity for electrode and getting better control of the electrochemical reactions.
The first part of this work studies the vibrational dynamics of aqueous Pt/CO interface using ab-initio molec-ular dynamics simulations. It presents the aqueous platinum interface with different CO adsorption coverage. The apparently simple and well-established system, however, involves an underlying physical complexity associated with the dynamic nature of solvent and adsorbates at the surface. Our simulations clarify the experimental observations.
The second part of this work focuses on the role of nuclear quantum effects at aqueous metal interfaces, illustrating the quantum dynamical behavior of water at metal interfaces. The results unambiguously show that quantum delocalization enhances ionization of water at aqueous platinum interface as compared to the aqueous gold interface, this effect not being captured by classical molecular dynamics. It reports extensive path-integral and classical ab-initio molecular dynamics simulations addressing the structural, electronic and electrochemical properties.
The last part reports long time-scale quantum dynamics of the bulk hydrated electron at the accuracy of many-body electronic structure theory. This result is achieved by training a machine learning potential capable of addressing dynamical, structural, and electronic properties of this unusual and important chemical species. Uncompromising description of electronic and nuclear quantum behavior of the system allows, for the first time, chemical accuracy for the modeling of a solvated electron and recovers most experimentally relevant observables, e.g. structural parameters of the cavity, vibrational spectra, diffusion dynamics. The quantum effects on nuclei revealed a novel diffusion mechanism that has not been observed in classical molecular dynamics and involves a twin-cavity intermediate.
The results from this thesis provide important details on the structural, dynamical and electronic properties of these important condensed aqueous systems. It also provides simulation protocols that allow the efficient sampling over long time scales with the help of advanced sampling methods or machine learning intermolecular potentials.
兰晶岗博士，苏黎世大学博士后。长期围绕计算机模拟固体界面，溶液复杂系统的核心问题展开研究，在Nature Communications, Journal of Physical Chemistry Letter, JACS, ACS Nano, Small, Journal of Physical Chemistry C等期刊发表10余篇。本科就读于华东理工大学应用化学系；硕士收到欧盟Erasmus Mundus全额奖学金于西班牙马德里自治大学，荷兰格罗宁根大学就读联合培养计算化学硕士；博士加入CP2K开发者小组（导师Prof. J. Hutter）于苏黎世大学攻读计算化学博士。