Structure and Dynamics of Strongly Interacting Systems in the Condensed Phase: From Glasses to Quantum Transport.

凝聚相强相互作用系统的结构和动力学：从玻璃到量子传输。

• 批准号: 1213247
• 负责人: David Reichman
• 金额: $ 42万
• 依托单位: Columbia University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2012
• 资助国家: 美国
• 起止时间: 2012-07-15 至 2015-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1213247&HistoricalAwards=false
• 关键词: Structure; Dynamics; Strongly; Interacting; Systems

David Reichman of Columbia University is supported by the Chemical Theory, Models and Computational Methods program to develop theoretical tools to investigate classical glassy liquids as well as quantum energy transfer and charge transport in condensed phase and nanoscale systems. In the first part of the program, new approaches are outlined to isolate and quantify growing structural order in supercooled liquids. The length scale associated with growing amorphous order is used to predict dynamical behavior in liquids as they approach the glass transition. In addition, the information obtained on a host of growing length scales (both structural and dynamic) is used to test and distinguish competing theories of the glass transition. In the second and third parts of the program novel methods are developed to describe real-time transport in condensed phase quantum systems. These methodologies include development of our RDM-Hybrid approach to understand energy and electron transfer in condensed media in the difficult cases of intermediate coupling germane to charge transport in organic crystals and aggregates, and a combination of our recent advance in electronic structure theory for strong static correlation (the DMFT for molecules approach) with our newly developed realtime "bold" Monte Carlo technique. This combination will allow, for the first time, a rigorous description of real-time quantum transport in driven systems where charge is transported through transition-metal containing clusters.In addition to the fundamental impact associated with a better understanding of the glass transition, the isolation and quantification of growing amorphous order may lead to better strategies for the design of targeted material properties in amorphous solids. The realistic description of transport properties in quantum condensed phase systems will have technological impact via a greater understanding of the fundamental events that underlie processes such as those that occur in solar energy conversion. In addition a program to communicate cutting edge science to high school students and the general public is being planned through collaboration with the New York Academy of Sciences.

哥伦比亚大学的大卫赖克曼得到化学理论、模型和计算方法项目的支持，开发理论工具来研究经典的玻璃态液体以及凝聚相和纳米级系统中的量子能量转移和电荷传输。在该计划的第一部分，概述了新的方法来隔离和量化过冷液体中不断增长的结构顺序。与成长无定形秩序的长度尺度被用来预测在液体中的动力学行为，因为它们接近玻璃化转变。此外，获得的信息上主机的增长长度尺度（结构和动态）用于测试和区分玻璃化转变的竞争理论。在程序的第二和第三部分中，开发了新的方法来描述凝聚相量子系统中的实时传输。这些方法包括我们的RDM-混合方法的发展，以了解在凝聚介质中的能量和电子转移的困难情况下，中间耦合密切相关的有机晶体和聚集体中的电荷传输，并结合我们最近的进展，在电子结构理论的强静态相关（DMFT分子的方法）与我们新开发的实时“大胆”蒙特卡罗技术。这种结合将允许，第一次，一个严格的描述，实时量子传输驱动系统中的电荷是通过过渡金属含clusters.In更好地理解玻璃化转变的基本影响，隔离和量化的增长无定形秩序可能会导致更好的策略，在无定形固体的目标材料性能的设计。量子凝聚相系统中传输特性的现实描述将通过更好地理解太阳能转换过程中发生的基本事件而产生技术影响。此外，通过与纽约科学院的合作，正在计划一个向高中生和公众传播尖端科学的方案。