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

拟议的研究包括对含有重金属的小分子的计算研究，这些小分子在通过精密光谱学寻找新物理中发挥重要作用，以及对极性分子的激光冷却的研究，这是原子、分子和光学物理领域的两个前沿领域。拟议的计算技术工作涉及开发新的算法和计算机程序，以提供增强的分子性质计算能力，这些性质与寻找电子电偶极矩(EEDM)和核磁四极矩(NMQM)有关，这是电子或原子核的本征性质，对于理解标准模型以外的新物理具有核心重要性。与实验小组密切合作提出的分子应用旨在提供对与激光冷却尖端研究和寻找新物理相关的分子的见解。本文提出的方法发展工作集中在一种分析方案，用于有效电场和T，P-奇相互作用的相对论耦合团簇计算，该T，P-奇相互作用与通过精确光谱搜索eEDM和NMQM有关。新的分析方案比目前使用电子能量数值微分的技术效率高一个数量级。除了提高效率外，所提出的分析方案还具有黑箱性质并且易于使用。这旨在为寻找新物理的候选分子的选择研究带来变革性的影响。这里提出的分子应用工作集中于对过渡金属和含有f元素的小分子的电子和振动性质的准确预测，包括自旋-轨道混合和Frank-Condon因子，以提供对它们在激光冷却和寻找eEDM中的应用的见解。物理部和化学部为这一奖项提供资金。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 of heavy-metal-containing small molecules that play important roles in the search for new physics via precision spectroscopy and research on laser cooling of polar molecules, two frontier areas in the field of atomic, molecular, and optical physics. The proposed work on computational techniques deals with the development of new algorithms and computer programs to provide enhanced capabilities for computations of molecular properties pertinent to the search for the electron electric dipole moment (eEDM) and the nuclear magnetic quadrupole moment (NMQM), intrinsic properties of an electron or nucleus of central importance to understanding new physics beyond the Standard Model. Proposed molecular applications in close collaboration with experimental groups aim to provide insights into molecules relevant to cutting-edge research in laser cooling and in search for new physics. The method-development work proposed here is focused on an analytic scheme for relativistic coupled-cluster calculations of effective electric field and the T, P-odd interaction pertinent to search of eEDM and NMQM via precision spectroscopy. The new analytic scheme is an order of magnitude more efficient than currently available techniques using numerical differentiation of electronic energies. In addition to improved efficiency, the proposed analytic scheme is also of a black-box nature and easy to use. This aims to bring a transformative impact to the research in the selection of candidate molecules for the search of new physics. The molecular application work proposed here is focused on accurate predictions of electronic and vibrational properties, including spin-orbit mixing and Franck-Condon factors, for transition-metal and f-element-containing small molecules to provide insights for their use in laser cooling and in the search for eEDM.The Physics Division and The Chemistry Division contribute funds to this award.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.