Ab-Initio Molecular Dynamics: Novel Developments with Application to H Bonded Systems

普林斯顿大学的Roberto Car获得了理论、模型和计算方法项目的奖励，以开发新的理论和计算增强的ab-initio分子动力学（AIMD）模拟，特别关注水和氢键系统的应用。PI和他的研究小组专注于一个四管齐下的战略：(i)基于包含色散力的更精确的电子密度函数的模拟将成为可能；（ii）利用一种新的理论概念，可以前所未有地比较量子模拟和深度非弹性中子散射数据，包括已经进行的和新计划的实验，从而揭示参与氢键的质子所经历的潜力；（iii）一种新的真实空间方案将被实施，以精确的多体方法（例如GW近似和Bethe-Salpeter方程）计算具有数百个原子的系统在AIMD模拟的选定快照中的核心和价电子激发，促进与实验（x射线，紫外线和光学光谱）及其解释的比较，以及（iv）疏水界面对水离子的亲和力将用热力学积分技术计算。促进对具有重大科学和技术意义的过程的分子水平的理解。该项目将通过分子模拟和光谱计算的新算法为科学基础设施做出贡献，这些算法将通过开放软件平台Quantum Espresso和Car-Parrinello分子动力学提供给更广泛的科学和工程界。这个项目的教育部分与拟议的研究很好地结合在一起。

Roberto Car of Princeton University is supported by an award from The Theory, Models and Computational Methods program to develop new theoretical and computational enhancements of ab-initio molecular dynamics (AIMD) simulations with special focus on applications to water and hydrogen-bonded systems. The PI and his research group focus on a four-pronged strategy: (i) simulations based on more accurate electronic density functional with inclusion of dispersion forces will be made possible, (ii) the potential experienced by the protons participating in hydrogen bonds will be unearthed by utilizing a novel theoretical concept that allows unprecedented comparison of quantum simulations and deep inelastic neutron scattering data, including already performed and newly planned experiments, (iii) a new real space scheme will be implemented to compute core and valence electronic excitations with accurate many-body methods (e. g. the GW approximation and the Bethe-Salpeter equation) for systems with hundreds of atoms at selected snapshots of AIMD simulations, boosting comparison with experiments (X-rays, UV and optical spectra) and their interpretation, and (iv) the affinity of hydrophobic interfaces for water ions will be computed with thermodynamic integration techniques, advancing the understanding at the molecular level of processes of great scientific and technological relevance.The project will contribute to the scientific infrastructure with new algorithms for molecular simulation and spectral calculation, which will be made available to the wider science and engineering community through the open software platforms Quantum Espresso and Car-Parrinello Molecular Dynamics. The educational component of this project is well integrated with the proposed research.