CAREER: Investigating the structure and dynamics of proton defects in heterogeneous environments with accelerated quantum simulations

职业：通过加速量子模拟研究异质环境中质子缺陷的结构和动力学

基本信息

批准号：
1652960
负责人：
Thomas Markland
金额：
$ 65.55万
依托单位：
Stanford University
依托单位国家：
美国
项目类别：
Continuing Grant
财政年份：
2016
资助国家：
美国
起止时间：
2016-12-01 至 2021-11-30
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1652960&HistoricalAwards=false
关键词：
CAREER Investigating structure dynamics proton

项目摘要

Thomas Markland of Stanford University is supported by an award from the Chemical Theory, Models and Computational Methods program to develop techniques to speed up molecular simulations. The particular focus is on transport of protons in complex environments. These simulations include the quantum mechanical nature of the electrons and nuclei that make up the atoms in a molecule. Markland's approach allows for making and breaking chemical bonds as the simulation progresses, which is essential for understanding the transport and chemical reactivity of light atoms such as protons. Proton transport processes in disordered systems are of fundamental importance in systems ranging from chemistry and materials science to geology and biology. These include the elucidation of transport mechanisms in proton exchange membranes used in fuel cells and in biological proton channels, providing insights into their functionality, and how to tune these materials for high efficiency proton transport. Professor Markland is also developing simulation and visualization experiences to improve high school education as well as to encourage more students to study chemistry by hosting high school teachers in his lab. These simulation and visualization experiences aid teachers in implementing scientific exercises that engage students' interest and stimulate them to inquire about the natural world. This is being achieved via partnership with several Stanford outreach programs. This research is aimed at understanding of the structure and dynamics of proton defects in heterogeneous environments, in concert with the development of approaches to accelerate ab initio path integral molecular dynamics simulations. These methods exploit time- and length-scale separation approaches to increase the efficiency of these simulations based on ring polymer contraction and multiple time-scale molecular dynamics algorithms. Markland and his research group use these approaches to investigate the interplay of structure and dynamics in a wide range of heterogeneous systems containing proton defects ranging from hydrophobic and hydrophilic interfaces to nanoporous systems. These studies are being used to understand how the chemical environment can be tailored to change the transport and reactivity of proton defects

斯坦福大学的托马斯·马克兰 (Thomas Markland) 获得了化学理论、模型和计算方法项目的奖项，以开发加速分子模拟的技术。特别关注复杂环境中质子的传输。这些模拟包括构成分子中原子的电子和原子核的量子力学性质。马克兰的方法允许随着模拟的进行形成和破坏化学键，这对于理解质子等轻原子的传输和化学反应性至关重要。无序系统中的质子传输过程对于从化学和材料科学到地质学和生物学的系统至关重要。其中包括阐明燃料电池和生物质子通道中使用的质子交换膜的传输机制，提供对其功能的深入了解，以及如何调整这些材料以实现高效质子传输。马克兰教授还在开发模拟和可视化体验，以改善高中教育，并通过在他的实验室接待高中教师来鼓励更多学生学习化学。这些模拟和可视化体验可帮助教师实施科学练习，激发学生的兴趣并激发他们对自然世界的探究。这是通过与斯坦福大学的几个外展项目合作实现的。这项研究旨在了解异质环境中质子缺陷的结构和动力学，同时开发加速从头算路径积分分子动力学模拟的方法。这些方法利用时间和长度尺度的分离方法来提高基于环聚合物收缩和多时间尺度分子动力学算法的模拟的效率。马克兰和他的研究小组使用这些方法来研究含有质子缺陷的各种异质系统中结构和动力学的相互作用，这些系统包括从疏水和亲水界面到纳米多孔系统。这些研究被用来了解如何调整化学环境来改变质子缺陷的传输和反应性

项目成果

期刊论文数量（12）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

i-PI 2.0: A universal force engine for advanced molecular simulations

i-PI 2.0：用于高级分子模拟的通用力引擎

DOI：
10.1016/j.cpc.2018.09.020
发表时间：
2018-08-11
期刊：
Comput. Phys. Commun.
影响因子：
0
作者：
V. Kapil;M. Rossi;O. Marsalek;Riccardo Petraglia;Y. Litman;Thomas Spura;Bingqing Cheng;Alice Cuzzocrea
通讯作者：
Alice Cuzzocrea

Hiding in the Crowd: Spectral Signatures of Overcoordinated Hydrogen-Bond Environments

隐藏在人群中：过度配位氢键环境的光谱特征

DOI：
10.1021/acs.jpclett.9b01781
发表时间：
2019-10
期刊：
The Journal of Physical Chemistry Letters
影响因子：
0
作者：
Morawietz, Tobias;Urbina, Andres S.;Wise, Patrick K.;Wu, Xiangen;Lu, Wanjun;Ben;Markland, Thomas E.
通讯作者：
Markland, Thomas E.

Resolving Heterogeneous Dynamics of Excess Protons in Aqueous Solution with Rate Theory

用速率理论解决水溶液中过量质子的非均相动力学

DOI：
10.1021/acs.jpcb.0c02649
发表时间：
2020-07
期刊：
The Journal of Physical Chemistry B
影响因子：
0
作者：
Roy, Santanu;Schenter, Gregory K.;Napoli, Joseph A.;Baer, Marcel D.;Markland, Thomas E.;Mundy, Christopher J.
通讯作者：
Mundy, Christopher J.

Nuclear quantum effects enter the mainstream

核量子效应进入主流