CDS&E: Development and applications of electronic structure methods for non-linear spectroscopy

南加州大学的Anna Krylov获得了化学学部化学理论、模型和计算化学项目的奖励，为非线性光学（NLO）特性建模开发了理论方法和强大的计算工具。CISE/ACI CIF21软件重用和计算与数据驱动科学与工程风险基金（CDS&amp；E）也为该奖项提供了资助。Krylov和她的研究小组正在开发形式和实现计算方法，以计算耦合簇（CC）和运动方程（EOM）系列方法中双光子吸收（2PA）的电子因子。这些发展扩展了稳健和准确的EOM- cc方法来描述EOM属性。为了使应用程序能够应用于现实系统（20-30个原子，~1000个基函数），他们利用了最近的方法、计算和软件开发。为了包括环境（如蛋白质、溶剂、分子固体）对NLO性质的影响，他们采用了有效片段电位。Krylov和同事正在应用这些新的计算工具来询问决定用于体内成像的荧光蛋白的2PA发色团亮度的因素。这项研究促进了对非线性过程的基本理解，这些过程在新的光谱方法和技术中得到了利用。在本研究框架内开发的计算机代码将广泛提供给研究社区，可用于设计更好的荧光标记，用于生物成像，研究活系统中的细胞过程，光动力疗法和生物传感器。这些工具还可用于开发用于微加工、3D光学数据存储和纳米光刻、超快速电光调制和开关以及各种其他新型纳米生物光子学应用的NLO材料。

Anna Krylov of the University of Southern California is supported by an award from the Chemical Theory, Models and Computational Chemistry program in the Chemistry Division to develop theoretical methods and robust computational tools for modeling non-linear optical (NLO) properties. The CISE/ACI CIF21 Venture Fund for Software Reuse and the Computational and Data-Enabled Science and Engineering (CDS&E) have also contributed to funding this award. Krylov and her research group are developing formalisms and implementing computational methods to compute electronic factors for two-photon absorption (2PA) within the coupled-cluster (CC) and equation-of-motion (EOM) family of methods. These developments extend the robust and accurate EOM-CC methodology to describe EOM properties. To enable applications to realistic systems (20-30 atoms, ~1000 basis functions), they capitalize on recent methodological, computational and software developments. To include the effect of the environment (e.g., protein, solvent, molecular solid) on NLO properties, they employ the Effective Fragment Potential. Krylov and coworkers are applying these new computational tools to interrogate factors determining 2PA brightness of chromophores of fluorescent proteins used for in vivo imaging. This research promotes fundamental understanding of non-linear processes that are exploited in novel spectroscopic approaches and technology. The computer codes developed in the framework of this research, which will be widely available to the research community, can used to design better fluorescent labels for using in bioimaging to study cellular processes in live systems, photodynamic therapy, and biosensors. These tools can also be used for developing NLO materials for micro-fabrication, 3D optical data storage and nanolithography, ultra-fast electro-optic modulation and switching, and a variety of other novel nano-bio-photonics applications.