A multireference coupled-cluster method for ground and excited states calculations of interstellar molecules

星际分子基态和激发态计算的多参考耦合簇方法

• 批准号: 1856702
• 负责人: Ludwik Adamowicz
• 金额: $ 43.5万
• 依托单位: University of Arizona
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-07-01 至 2025-01-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1856702&HistoricalAwards=false
• 关键词: multireference; coupled; cluster; method; ground

Professor Ludwik Adamowicz of the University of Arizona is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry. His project is based on using fundamental principles of quantum mechanics (QM) in predicting chemical and physical properties of primordial molecular systems. Some of these molecules, for example, the simplest triatomic ion H3+, has played a pivotal role in the evolution of our universe. Professor Adamowicz's QM calculations will use the most powerful present-day computers to provide results pertaining to the spectral transitions and chemical behavior of molecules relevant to experimental astrochemical/astrophysical research. The major effort in this research will go to the development of new QM computational methods whose accuracy matches or even exceeds the accuracy of present-day experimental measurements. Most of our knowledge of the astronomical world is derived from the absorption, emission and scattering of electromagnetic radiation from atoms and molecules. Astronomical observations of atomic and molecular spectra, including transition energies, intensities, and light polarization, complement both laboratory experiments and the new theoretical calculations from the Adamowicz group to develop a better understanding of stellar atmospheres and their evolutions. Professor Adamowicz will engage both science and non-science undergraduate students in the application of modern computational methods. He makes the new software developed in this project available to the broader scientific community.Professor Adamowicz and his group are developing new methods that utilize first-principles quantum mechanics to study chemical and physical properties of small and medium-size molecular systems in the gas phase. The methods are expected to elevate the predictive capability of computational quantum chemistry to a level of accuracy unattainable using present-day approaches. The first focus is on an active-space multireference coupled-cluster method that can be applied to study molecules in their ground and excited states at and away from their equilibrium structures. The second focus is on developing methods for performing molecular calculations with all-electron explicitly correlated Gaussian (ECG) functions. Methods based on the Born-Oppenheimer (BO) approximation and non-BO methods are also being developed. The ECGs are implemented in rovibrational calculations. Professor Adamowicz and his group are applying the new methods to study properties and spectra of various molecular systems such as HCO+, CH5+, H3+, HeH2+, HeH, LiHe+, BeH+, LiH2+, etc.. These are all important to the interstellar chemistry of the universe from its primordial stages to the present.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.

亚利桑那大学的Ludwik Adamowicz教授获得了化学系化学理论，模型和计算方法项目的奖项。 他的项目是基于使用量子力学（QM）的基本原理来预测原始分子系统的化学和物理性质。其中一些分子，例如最简单的三原子离子H3+，在我们宇宙的演化中发挥了关键作用。Adamowicz教授的QM计算将使用当今最强大的计算机来提供与实验天体化学/天体物理研究相关的分子的光谱跃迁和化学行为有关的结果。在这项研究中的主要努力将去开发新的QM计算方法，其准确性匹配，甚至超过了当今的实验测量的准确性。我们对天文世界的大部分知识都来自原子和分子对电磁辐射的吸收、发射和散射。原子和分子光谱的天文观测，包括跃迁能量、强度和光偏振，补充了实验室实验和Adamowicz小组的新理论计算，以更好地理解恒星大气及其演变。 教授Adamowicz将从事科学和非科学本科学生在现代计算方法的应用。 Adamowicz教授和他的团队正在开发新的方法，利用第一性原理量子力学来研究气相中小分子和中等分子系统的化学和物理性质。这些方法有望将计算量子化学的预测能力提升到使用当今方法无法达到的准确度水平。第一个重点是一个积极的空间多参考耦合集群方法，可应用于研究分子在其基态和激发态，并远离其平衡结构。第二个重点是开发方法进行分子计算与全电子显式相关高斯（ECG）功能。基于Born-Oppenheimer（BO）近似和非BO方法的方法也正在开发中。在振转计算中实现ECG。Adamowicz教授和他的团队正在应用新方法研究各种分子体系的性质和光谱，如HCO+，CH 5+，H3+，HeH 2+，HeH，LiHe+，BeH+，LiH 2+等。 这一奖项反映了NSF的法定使命，并通过使用基金会的知识价值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

A quantum-mechanical non-Born–Oppenheimer model of a molecule in a strong magnetic field

强磁场中分子的量子力学非玻恩奥本海默模型

• DOI: 10.1016/j.cplett.2020.138041
• 发表时间: 2020
• 期刊: Chemical Physics Letters
• 影响因子: 2.8
• 作者: Adamowicz, Ludwik;Stanke, Monika;Tellgren, Erik;Helgaker, Trygve
• 通讯作者: Helgaker, Trygve

Fine structure of the beryllium P3 states calculated with all-electron explicitly correlated Gaussian functions

用全电子显式相关高斯函数计算铍 P3 态的精细结构

• DOI: 10.1103/physreva.105.012813
• 发表时间: 2022
• 期刊: Physical Review A
• 影响因子: 2.9
• 作者: Stanke, Monika;Kędziorski, Andrzej;Adamowicz, Ludwik
• 通讯作者: Adamowicz, Ludwik

Fine structure of the P2 energy levels of singly ionized carbon (C ii)

单电离碳 (C ii) P2 能级的精细结构

• DOI: 10.1103/physreva.108.012812
• 发表时间: 2023
• 期刊: Physical Review A
• 影响因子: 2.9
• 作者: Stanke, Monika;Kędziorski, Andrzej;Nasiri, Saeed;Adamowicz, Ludwik;Bubin, Sergiy
• 通讯作者: Bubin, Sergiy

Low-lying S2 states of the singly charged carbon ion

单电荷碳离子的低位 S2 态

• DOI: 10.1103/physreva.102.062825
• 发表时间: 2020
• 期刊: Physical Review A
• 影响因子: 2.9
• 作者: Hornyák, István;Adamowicz, Ludwik;Bubin, Sergiy
• 通讯作者: Bubin, Sergiy

Oscillator strengths and interstate transition energies involving 2S and 2P states of the Li atom

涉及 Li 原子 2S 和 2P 态的振荡器强度和态间跃迁能量

• DOI: 10.1016/j.adt.2022.101559
• 发表时间: 2023
• 期刊: Atomic Data and Nuclear Data Tables
• 影响因子: 1.8
• 作者: Nasiri, Saeed;Liu, Jian;Bubin, Sergiy;Stanke, Monika;Kȩdziorski, Andrzej;Adamowicz, Ludwik
• 通讯作者: Adamowicz, Ludwik