New Coupled-cluster Methods for Linear and Non-linear Valence and Core-level Spectroscopy in Gas and Condensed Phase

气相和凝聚相中线性和非线性价态和核心级光谱学的新耦合簇方法

• 批准号: 2154482
• 负责人: Anna Krylov
• 金额: $ 51万
• 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: 2022
• 资助国家: 美国
• 起止时间: 2022-05-15 至 2025-04-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2154482&HistoricalAwards=false
• 关键词: New; Coupled; cluster; Methods; Linear

Anna Krylov of the University of Southern California is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to develop new theoretical approaches, computer algorithms, and software to describe interaction of molecules and light in new regimes (high energy, high intensities, etc). Using light to interrogate matter is the basis of spectroscopy, which provides the most powerful set of tools for unraveling mechanisms of chemical reactions, structures and intrinsic properties of materials and biological objects. Using high-energy (X-rays) and high-intensity radiation opens new exciting opportunities, which motivate the worldwide development of multi-billion facilities for advanced light sources. Recent advances in beam quality in these facilities greatly expanded possible applications of X-rays, giving rise to a proliferation of techniques including those operating in time-resolved and non-linear regimes. These novel techniques promise to greatly expand our ability to interrogate molecular structure and dynamics, but their full potential can only be realized when experiment is augmented by accurate theoretical tools for modeling these phenomena. Despite significant efforts, the theory is still lagging behind the experimental capabilities, creating a bottleneck for maximizing the scientific impact of multi-billion advanced light source facilities. Krylov will bridge this gap by developing novel electronic structure methods for modeling linear and non-linear core-level spectroscopies in the gas and condensed phases. The research plans include training and mentoring of graduate students and postdocs for careers in academia and industry as well as contributions to the research infrastructure.Capitalizing on her previous work, Krylov will further extend highly reliable coupled-cluster (CC) and equation-of-motion CC (EOM-CC) methods to the domain of core-level ionized and excited states by exploiting core-valence separation (CVS) and damped response theory (or complex polarization propagator, CPP) approaches. Specifically, she will further develop theoretical framework and efficient computer codes for modeling E2PA (entangled 2PA), PECD (photoelectron circular dichroism), MCD (magnetic CD), and electronic SFG (sum-frequency generation) spectra. She aims to develop a uniform theoretical framework for both UV–vis (valence transitions) and X-ray (core-level transitions) domains. Continuing close collaborations with experimentalists guides and calibrate the developments, as well as helps to design new experiments and interpret the experimental results.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.

南加州大学的 Anna Krylov 获得化学系化学理论、模型和计算方法项目的奖项支持，以开发新的理论方法、计算机算法和软件来描述新体系中分子和光的相互作用（利用光来探究物质是光谱学的基础，它为揭示高能材料和生物物体的化学反应、结构和内在性质的机制提供了最强大的工具。 （X 射线）和高强度辐射开辟了新的令人兴奋的机会，推动了全球数十亿美元的先进光源设施的开发，这些设施光束质量的最新进展极大地扩展了 X 射线的可能应用，从而产生了技术的激增，包括在时间分辨和非线性状态下运行的技术，这些新技术有望极大地扩展我们研究分子结构和动力学的能力，但只有通过精确的理论工具来增强实验，才能充分发挥它们的潜力。对这些现象进行建模。克雷洛夫将通过开发新颖的电子结构方法来弥补这一差距，用于模拟气体和凝聚阶段的线性和非线性核心级光谱。研究计划包括对研究生和博士后在学术界和工业界的职业生涯进行培训和指导。对研究基础设施的贡献。利用她之前的工作，克雷洛夫将进一步扩展通过利用核价分离 (CVS) 和阻尼响应理论（或复极化传播器），在核级电离态和激发态域中采用高度耦合团簇 (CC) 和可靠的运动方程 CC (EOM-CC) 方法具体来说，她将进一步开发用于建模 E2PA（纠缠 2PA）、PECD（光电子圆二色性）、MCD（磁性 CD）和电子 SFG 的理论框架和高效计算机代码。 （和频生成）光谱。她的目标是为 UV-vis（价态跃迁）和 X 射线（核心能级跃迁）领域开发统一的理论框架，并继续与实验学家密切合作，指导和校准发展。有助于设计新的实验并解释实验结果。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力优点和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

DFT exchange: sharing perspectives on the workhorse of quantum chemistry and materials science.

• DOI: 10.1039/d2cp02827a
• 发表时间: 2022-12-07
• 期刊: PHYSICAL CHEMISTRY CHEMICAL PHYSICS
• 影响因子: 3.3
• 作者: Teale, Andrew M.;Helgaker, Trygve;Savin, Andreas;Adamo, Carlo;Aradi, Balint;Arbuznikov, Alexei, V;Ayers, Paul W.;Baerends, Evert Jan;Barone, Vincenzo;Calaminici, Patrizia;Cances, Eric;Carter, Emily A.;Chattaraj, Pratim Kumar;Chermette, Henry;Ciofini, Ilaria;Crawford, T. Daniel;De Proft, Frank;Dobson, John F.;Draxl, Claudia;Frauenheim, Thomas;Fromager, Emmanuel;Fuentealba, Patricio;Gagliardi, Laura;Galli, Giulia;Gao, Jiali;Geerlings, Paul;Gidopoulos, Nikitas;Gill, Peter M. W.;Gori-Giorgi, Paola;Gorling, Andreas;Gould, Tim;Grimme, Stefan;Gritsenko, Oleg;Jensen, Hans Jorgen Aagaard;Johnson, Erin R.;Jones, Robert O.;Kaupp, Martin;Koster, Andreas M.;Kronik, Leeor;Krylov, Anna, I;Kvaal, Simen;Laestadius, Andre;Levy, Mel;Lewin, Mathieu;Liu, Shubin;Loos, Pierre-Francois;Maitra, Neepa T.;Neese, Frank;Perdew, John P.;Pernal, Katarzyna;Pernot, Pascal;Piecuch, Piotr;Rebolini, Elisa;Reining, Lucia;Romaniello, Pina;Ruzsinszky, Adrienn;Salahub, Dennis R.;Scheffler, Matthias;Schwerdtfeger, Peter;Staroverov, Viktor N.;Sun, Jianwei;Tellgren, Erik;Tozer, David J.;Trickey, Samuel B.;Ullrich, Carsten A.;Vela, Alberto;Vignale, Giovanni;Wesolowski, Tomasz A.;Xu, Xin;Yang, Weitao
• 通讯作者: Yang, Weitao

How Reproducible Are QM/MM Simulations? Lessons from Computational Studies of the Covalent Inhibition of the SARS-CoV-2 Main Protease by Carmofur

• DOI: 10.1021/acs.jctc.2c00286
• 发表时间: 2022-07-07
• 期刊: JOURNAL OF CHEMICAL THEORY AND COMPUTATION
• 影响因子: 5.5
• 作者: Giudetti, Goran;Polyakov, Igor;Krylov, Anna I.
• 通讯作者: Krylov, Anna I.

Influence of Transition Metal Electron Configuration on the Structure of Metal–EDTA Complexes

过渡金属电子构型对金属-EDTA配合物结构的影响

• DOI: 10.1021/acs.jpca.2c07996
• 发表时间: 2023
• 期刊: The Journal of Physical Chemistry A
• 作者: Foreman, Madison M.;Alessio, Maristella;Krylov, Anna I.;Weber, J. Mathias
• 通讯作者: Weber, J. Mathias

Signatures of the Bromine Atom and Open-Shell Spin Coupling in the X-ray Spectrum of the Bromobenzene Cation

溴苯阳离子 X 射线谱中溴原子和开壳层自旋耦合的特征

• DOI: 10.1021/jacs.2c12334
• 发表时间: 2023
• 期刊: Journal of the American Chemical Society
• 影响因子: 15
• 作者: Epshtein, Michael;Tenorio, Bruno Nunes;Vidal, Marta L.;Scutelnic, Valeriu;Yang, Zheyue;Xue, Tian;Krylov, Anna I.;Coriani, Sonia;Leone, Stephen R.
• 通讯作者: Leone, Stephen R.

The Auger spectrum of benzene

苯的俄歇光谱

• DOI: 10.1063/5.0138674
• 发表时间: 2023
• 期刊: The Journal of Chemical Physics
• 作者: Jayadev, Nayanthara K.;Ferino-Pérez, Anthuan;Matz, Florian;Krylov, Anna I.;Jagau, Thomas-C.
• 通讯作者: Jagau, Thomas-C.