Accurate Electronic and Vibrational Structure Calculations of Metal-Containing Small Molecules of Importance to Precision Measurement and Laser Cooling

提议的研究包括计算研究，以描述小金属分子中电子和原子核的复杂运动，这些运动在寻找超越标准模型的新物理和新兴的量子信息科学中发挥重要作用。在计算技术方面的工作重点是开发新的算法和计算机程序，以阐明电子状态之间的微妙耦合在激光冷却分子到超冷温度中的作用。与实验小组密切合作提出的分子应用旨在提供与量子科学前沿研究和新物理学研究相关的分子见解。本文提出的方法发展工作集中在相对论耦合团簇理论上，以加强对含重原子分子激光冷却的重要非绝热效应的处理，并提高对电子电偶极矩的精确测量重要的有效电场的计算能力。拟议的应用工作包括对激光可冷却线性多原子分子的强度借入机制进行深入研究，并预测含金属小分子（包括RaOH， ThF+和YbOH）的性质，与致力于这些分子的激光冷却和精密光谱的实验小组密切合作。该奖项反映了美国国家科学基金会的法定使命，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。

The proposed research consists of computational studies to describe the complex motions of electrons and nuclei in small metal-containing molecules that play important roles in searching for new physics beyond the Standard Model and in the emerging quantum information sciences. The proposed work on computational techniques is focused on the development of new algorithms and computer programs to elucidate the roles of subtle coupling between electronic states in laser cooling of molecules to ultracold temperature. The proposed molecular applications in close collaboration with experimental groups aim to provide insights into molecules relevant to cutting-edge research in quantum sciences and in searches for new physics. The method-development work proposed here is focused on relativistic coupled-cluster theory to enhance the treatment of nonadiabatic effects of importance to laser cooling of molecules containing heavy atoms and to improve the ability to calculate effective electric fields of importance to precision measurement of the electron’s electric dipole moment (eEDM). The proposed application work consists of a thorough investigation of the intensity-borrowing mechanisms in laser-coolable linear polyatomic molecules and predictions of properties for metal-containing small molecules including RaOH, ThF+, and YbOH, in close collaboration with experimental groups working on laser cooling and precision spectroscopy of these molecules.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.