Exploring Response Properties of Molecules and Extended Systems Using Theoretical Methods

在化学系化学结构、动力学和机制(CSDM-A)计划的支持下，纽约州立大学布法罗分校的Jochen Autschbach教授将开发量子理论方法并进行大规模计算机模拟，以了解分子结构、化学键和分子运动如何决定可在实验中测量的各种分子性质。该项目将促进对分子结构和所测量的分子性质之间关系的理解。此外，这些研究可能有助于更好地理解光和物质之间的相互作用。该项目将为研究生和本科生提供培训，并为高中生提供暑期实习机会，例如在科学计算机编程方面。该项目的重点是分子性质，这些性质在了解分子的结构和功能以及化学系统的动力学方面具有很高的实用价值。理论发展和模拟将是建立和完善结构-财产关系的关键。该项目将特别关注核磁共振弛豫现象，以及光学活性的结构和电子起源。此外，还将通过计算来研究一类特殊有机自由基的行为，并辅之以由Pi Autschbach的合作者进行的实验。自由基对单个和最高占位的分子轨道进行了能量反转，引起了材料科学及相关领域的广泛关注。具体地说，对显示PI术语SOMO-HOMO反转的自由基的研究提供了一个有趣的基础研究领域；与合成化学家的合作将允许检查/验证计算预测。计划研究的另一个重要方面与核磁共振弛豫有关。核磁共振弛豫包含有关化学体系的动力学和特征动态时间尺度的丰富信息。弛豫将通过从头算和力场分子动力学模拟来预测。该项目与光学活动相关的部分将集中在拉曼振动光学活动、圆偏振发光和磁场诱导光学活动中的共振效应。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

With support from the Chemical Structure, Dynamics, and Mechanisms-A (CSDM-A) program of the Chemistry Division, Professor Jochen Autschbach of the University at Buffalo, State University of New York, will develop quantum theoretical methods and perform large-scale computer simulations, to learn how molecular structure, chemical bonding, and molecular motion determine a variety of molecular properties that can be measured in experiments. The project will advance the understanding of the relationships between molecular structure and measured properties of molecules. Furthermore, these studies will likely contribute to a better understanding of the interactions between light and matter. The project will provide training for graduate and undergraduate students and opportunities for summer internships of high school students, for example, in scientific computer programming. The project focuses on molecular properties that are of high practical value in informing about the structures and functions of molecules, and the dynamics of chemical systems. The theory developments and simulations will be crucial to establish and refine the sought-after structure-property relationships. The project will focus specifically on NMR relaxation phenomena, and on the structural and electronic origins of optical activity. In addition, the behavior of a special class of organic radicals will be studied by calculations, complemented by experiments performed by PI Autschbach’s collaborators. The radicals show an energetic inversion of the singly and the highest occupied molecular orbital, which has attracted much interest in materials science and related fields. Specifically, the investigation of radicals that display what the PI terms SOMO-HOMO inversion provides an interesting area of fundamental research; collaborations with synthetic chemists will allow for examination/validation of the computational predictions. Another important aspect of the planned studies relates to NMR relaxation. NMR relaxation contains a wealth of information about the dynamics and the characteristic dynamic time scales of a chemical system. Relaxation will be predicted by ab-initio and force-field molecular dynamics simulations. The optical activity-related part of the project will focus on resonance effects in Raman vibrational optical activity, circularly polarized luminescence, and magnetic-field induced optical activity.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.