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在化学理论、模型和计算方法计划的支持下开发了理论工具，以研究经典玻璃液体以及凝聚相和纳米级系统中的量子能量转移和电荷转移。在该计划的第一部分，概述了分离和量化过冷液体中不断增长的结构有序性的新方法。与无定形有序生长相关的长度尺度被用来预测液体在接近玻璃化转变时的动力学行为。此外，在一系列不断增长的长度尺度上获得的信息(包括结构和动态)被用来测试和区分相互竞争的玻璃化转变理论。在程序的第二部分和第三部分中，发展了描述凝聚相量子系统中实时输运的新方法。这些方法包括开发我们的RDM混合方法，以在中间耦合与有机晶体和聚集体中的电荷传输相关的困难情况下了解凝聚介质中的能量和电子转移，以及将我们最近在强静态关联电子结构理论方面的进展(分子的DMFT方法)与我们新开发的实时“BOLD”蒙特卡罗技术相结合。这一结合将首次实现对驱动系统中实时量子传输的严格描述，其中电荷通过含有过渡金属的团簇进行传输。除了与更好地理解玻璃转变相关的基本影响外，分离和量化生长的非晶态有序可能会导致更好地设计非晶态固体中的目标材料性质。对量子凝聚相系统中输运性质的真实描述将通过更好地理解过程中的基本事件，例如发生在太阳能转换中的过程，而产生技术影响。此外，正在计划通过与纽约科学院的合作，向高中生和普通公众传播尖端科学。

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.