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

拟议的研究包括描述含有金属的小分子中电子和原子核的复杂运动的计算研究，这些小分子在寻找超越标准模型的新物理和在新兴的量子信息科学中发挥重要作用。计算技术方面的工作集中在开发新的算法和计算机程序，以阐明电子态之间的微妙耦合在分子激光冷却到超冷温度中的作用。拟议中的分子应用与实验小组密切合作，旨在提供对与量子科学尖端研究和新物理搜索相关的分子的见解。本文提出的方法发展工作集中在相对论耦合团簇理论，以加强对含有重原子的分子的激光冷却的重要的非绝热效应的处理，并提高计算对精确测量电子的电偶极矩(EEDM)具有重要意义的有效电场的能力。拟议的申请工作包括彻底调查激光可冷却的线性多原子分子中的强度借用机制，并与从事激光冷却和这些分子的精密光谱工作的实验小组密切合作，预测含金属小分子的性质，包括RaOH，THF+和YbOH。这一奖项反映了NSF的法定使命，并通过使用基金会的智力优势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.