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

哥伦比亚大学的David Reichman得到了化学理论、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液体，以及凝聚态和纳米级系统中的量子能量转移和电荷输运。在该计划的第一部分，新方法概述了隔离和量化在过冷液体增长的结构秩序。长度尺度与生长的无定形秩序是用来预测动力学行为的液体，因为他们接近玻璃化转变。此外，在大量不断增长的长度尺度（结构和动态）上获得的信息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，开发了描述凝聚相量子系统中的实时输运的新方法。这些方法包括我们的RDM-Hybrid方法的发展，以理解在有机晶体和聚集体中与电荷输运相关的中间耦合困难情况下凝聚态介质中的能量和电子转移，以及我们在强静态相关电子结构理论（分子DMFT方法）方面的最新进展与我们新开发的实时“大胆”蒙特卡罗技术的结合。这种结合将首次允许对驱动系统中的实时量子输运进行严格描述，其中电荷通过包含过渡金属的簇进行输运。除了与更好地理解玻璃化转变相关的基本影响外，非晶有序生长的分离和量化可能会为非晶固体中目标材料性能的设计提供更好的策略。对量子凝聚相系统中输运性质的现实描述，将通过对太阳能转换等过程中发生的基本事件的更深入理解，对技术产生影响。此外，通过与纽约科学院合作，正在计划一个向高中生和公众传播尖端科学的项目。

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.