Molecular Quantum Control Within the Frequency Domain

这个项目连接了三个传统上分离的研究领域：分子光谱学、量子光学和相干控制。这里使用的频域量子控制工具不同于相干控制中使用的时域控制方案。近年来，该工具被用于证明分子角动量控制和高精度测量分子跃迁偶极矩矩阵元的绝对大小，它在分子吸收和发射光中起着至关重要的作用。本计划的目标是为频域控制方案开发分子动力学应用。除了正在进行的量子控制研究外，本项目将尝试控制分子的预解离，并研究价电子自旋在反应性碰撞中的作用。本项目还涉及对超冷分子物理感兴趣的分子结构的研究。频域控制方案与四色激发方案相结合，可用于分子种群的状态选择性转移到电子基态的最低振动水平，这一过程对于涉及光学晶格中超冷分子的应用至关重要。此外，本项目还包括碱二聚体的三重态基态和第一激发态电位的实验测定。这些数据对研究超冷分子的形成具有重要意义。更广泛的影响包括与超冷分子工作的联系，并为分子量子光学的学生提供研究机会和指导。该项目还将继续为扩大代表性不足的研究生和本科生的参与作出有力贡献。

This project bridges three traditionally separated research areas: molecular spectroscopy, quantum optics and coherent control. The frequency domain quantum control tool used here differs from the time domain control schemes used in coherent control. Recently this tool has been used to demonstrate molecular angular momentum control and to measure with high accuracy the absolute magnitude of the molecular transition dipole moment matrix element, which plays a critical role in absorption and emission of light by molecules. The goal of this project is to develop molecular dynamics applications for the frequency domain control scheme. In addition to the ongoing research on quantum control, this project will attempt control of pre-dissociation of molecules, and study the role of valence electron spin in reactive collisions. This project also involves research on molecular structure of interest for ultracold molecular physics. The frequency domain control scheme, combined with a four color excitation scheme, can be used for state selective transfer of molecular population to the lowest vibrational levels of the electronic ground state, a process that is critical for applications involving ultracold molecules in optical lattices. In addition, the project includes an experimental determination of the triplet ground state and first excited states potentials of alkali dimers. These data will be important for research on ultracold molecule formation. Broader impacts include the connection with work on ultracold molecules and providing research opportunities and mentoring for students in molecular quantum optics. The project will also continue to contribute strongly to broadening the participation of underrepresented students, both graduate and undergraduate.