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

拟议的研究包括计算研究，以描述含金属的小分子中电子和原子核的复杂运动，这些分子在寻找标准模型之外的新物理学和新兴的量子信息科学中发挥着重要作用。拟议的计算技术的工作集中在新的算法和计算机程序的开发，以阐明激光冷却分子到超冷温度的电子状态之间的微妙耦合的作用。与实验小组密切合作的拟议分子应用旨在提供与量子科学前沿研究和寻找新物理学相关的分子的见解。 这里提出的方法开发工作的重点是相对论耦合集群理论，以提高治疗的非绝热效应的重要性，激光冷却的分子中含有重原子，并提高计算有效电场的能力，重要的是精确测量的电子的电偶极矩（eEDM）。拟议的应用工作包括对激光可冷却线性多原子分子中强度借用机制的彻底调查和对含金属小分子（包括RaOH、ThF+和YbOH）的性质的预测，该奖项反映了NSF的法定使命，并通过评估被认为值得支持使用基金会的知识价值和更广泛的影响审查标准。

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.