Ab initio method development for mechanistic studies of charge transport

电荷传输机理研究的从头算方法开发

• 批准号: 0951634
• 负责人: Anna Krylov
• 金额: $ 43.5万
• 依托单位: University of Southern California
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2010
• 资助国家: 美国
• 起止时间: 2010-09-01 至 2013-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0951634&HistoricalAwards=false
• 关键词: Ab; initio; method; development; mechanistic

Anna Krylov of the University of Southern California is supported by an award from the Theory, Models and Computational Methods program to develop predictive ab initio methods to characterize the electronic structure of ionized and electron-attached states in model systems, such as small clusters of nucleobases, DNA hairpins or similar systems. The proposed developments are based on the equation-of-motion coupled-cluster approach for ionization potentials (EOM-IP) and electron-attached (EOM-EA) systems, which is capable of describing multiple closely lying electronic states in an accurate, robust and efficient computational scheme The PI and her research group are (i) implementing properties and analytic gradient calculations for EOM-IP-CCSD using a Frozen Natural Orbitals (FNO) approach); (ii) implementing non-iterative triples corrections for the IP-CCSD and IP-CISD methods to improve accuracy of these methods; (iii) extending the FNO scheme to EOM-EA-CCSD energies and gradient calculations; (iv) implementing efficient calculations of Dyson orbitals and other inter-state properties to aid interpretation of the results and facilitate more direct comparisons with the experiments; and (v) parallelizing and redesigning the tensor library to take advantage of modern computer architecture.The Krylov group develops methods with the aim to study charge transport through molecular wires, which plays a central role in many important processes such as the radiative or oxidative damage in DNA, light harvesting, molecular electronics and solar energy applications. Software developed by this research group is made available to the community by being implemented in widely used software packages: Q-CHEM and SPARTAN.This award is supported partially by a co-funding arrangement with the Office of Cyberinfrastructure (OCI).

南加州大学的 Anna Krylov 获得理论、模型和计算方法计划奖项的支持，开发预测性从头算方法来表征模型系统中电离和电子附着态的电子结构，例如小核碱基簇、DNA发夹或类似系统。 所提出的进展基于电离势（EOM-IP）和电子附着（EOM-EA）系统的运动方程耦合簇方法，该方法能够以准确、鲁棒的方式描述多个紧密相连的电子态。和高效的计算方案 PI 和她的研究小组正在 (i) 使用冻结自然轨道 (FNO) 方法实现 EOM-IP-CCSD 的属性和解析梯度计算； (ii) 对 IP-CCSD 和 IP-CISD 方法实施非迭代三元组校正，以提高这些方法的准确性； (iii) 将 FNO 方案扩展到 EOM-EA-CCSD 能量和梯度计算； (iv) 对戴森轨道和其他态间特性进行有效计算，以帮助解释结果并促进与实验进行更直接的比较； (v) 并行化和重新设计张量库以利用现代计算机体系结构。Krylov 小组开发的方法旨在研究通过分子线的电荷传输，分子线在许多重要过程中发挥着核心作用，例如辐射或氧化损伤DNA、光捕获、分子电子学和太阳能应用。该研究小组开发的软件通过广泛使用的软件包 Q-CHEM 和 SPARTAN 向社区提供。该奖项部分由与网络基础设施办公室 (OCI) 的共同资助安排支持。