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.

南加州大学的安娜·克里洛夫（Anna Krylov）得到了化学理论，模型和计算方法计划的奖项，以开发新的理论方法，计算机算法和软件，以描述分子与光的相互作用在新制度（高能，高强度等）中的相互作用。使用光进行审问是光谱的基础，该光谱学为揭示化学反应，结构和材料和生物学对象的内在特性的机制提供了最强大的工具。使用高能量（X射线）和高强度辐射开辟了新的激动人心的机会，这激发了全球范围内数十亿个设施的高级光源的开发。这些设施中光束质量的最新进展极大地扩展了X射线的可能应用，从而引起了技术的扩散，包括在时间分辨和非线性方案中运行的技术。这些新颖的技术有望大大扩展我们询问分子结构和动力学的能力，但是只有当实验通过准确的理论工具来建模这些现象时，才能实现它们的全部潜力。尽管做出了巨大的努力，但该理论仍然落后于实验能力，从而创造了一种瓶颈，以最大程度地提高数十亿个高级光源设施的科学影响。克里洛夫（Krylov）将通过开发新型的电子结构方法来弥合这一差距，以建模气体和冷凝相中的线性和非线性核心水平光谱。研究计划包括对学术界和行业职业的研究生和博士后的培训和心理，以及对研究基础架构的贡献。对她先前的工作进行资本化，Krylov将进一步将高度可靠的耦合群集（CC）（CC）和动机cc（EOM-CC）进行核心（EOM-CC）的核心核心（EOM-CC），并将核心的核心核心核心发展扩展到核心的核心。以及据称的响应理论（或复杂的极化传播器，CPP）方法。具体而言，她将进一步开发理论框架和有效的计算机代码，用于建模E2PA（纠缠2PA），PECD（Photelectron圆形二科主义），MCD（磁性CD）和电子SFG（总频率生成）光谱。她的目标是为UV-VIS（Valence Transitions）和X射线（核心级过渡）域开发一个统一的理论框架。继续与实验者指南进行密切合作，校准发展，并有助于设计新的实验并解释实验结果。该奖项反映了NSF的法定任务，并通过使用该基金会的知识分子优点和更广泛的影响来评估NSF的法定任务，并被认为是宝贵的支持。

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.